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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Bubble Mass Transport Measurement in the Large-Scale Test Loops at Oak Ridge National Laboratory

Molten salts are complex fluids that incorporate multi-phase behavior depending on the chemistry and the physical properties of the entrained components. These components include the carrier salt, the actinide fuel, and fission, activation, and corrosion products, the concentrations of which depends on the burnup history of the salt. Radionuclide transport from the salt into the cover gas / off-gas system depends on volatility as predicted by thermochemistry, but data from the Molten Salt Reactor Experiment (MSRE) conducted in the late 1960s suggest that bubble formation and transport are also important. Anomalously high fractions of noble metals were found in the off-gas system and were attributed to transportation with parent salt aerosols and their association with rising noble gas bubbles. The prediction of such phenomena requires coupled neutronic, thermal hydraulic, and chemical equilibrium calculations, the framework of which is being developed within the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program supported by the US Department of Energy (DOE) Office of Nuclear Energy (NE). However, separate effects tests and models of experiments using tools such as SAM and Thermochimica can guide model developers through important processes. Conversely, model development guides the choice of experiments and systems to provide data that are relevant for validation. This report describes several experiments that tracked gas transport in molten salts, ranging from small-scale systems to large-scale loops. Gas transportation in a molten salt, LiCl-KCl, has been studied using the shadowgraph technique. Sensors such as residual gas analysis, Raman spectroscopy, and laser-induced breakdown spectroscopy have been tested for off-gas measurements. These data were used to interpret how the gases move through the upstream salt / cover gas and the interface between them. Differential pressure measurements were able to detect individual gas bubbles as they popped at the liquid–gas interface. Salt aerosols were collected on a cascade impactor. Their formation was also observed directly via the shadowgraph method, and most of these aerosols were launched ballistically into the cover gas. Fine mists could also be observed. Convection currents through the salt were visualized and can be used to calculate the thermophysical properties of the salt itself. The apparatuses described in this report and in a previous work (McFarlane et al. 2023) have been commissioned and are available for use in making further measurements of salt/surrogate fission product behavior. Novel approaches using neutron imaging are planned for the study of fluoride salts, which cannot be contained in quartz, so shadowgraph visualization is not available. Bubble transport in convective flow and in a slow-moving salt column are planned. The mobile laser-induced breakdown spectroscopy (LIBS) system is available for several applications, including iodine capture in a molten hydroxide scrubber, H2 transport though molten salts to complement Raman analysis, and online tracking of salt aerosol generation, transport, and deposition. This report summarizes the findings from FY24 and the plans for FY25. The work completes milestone M2AT-24OR0702013 of the DOE-NE Advanced Reactor Technology, Molten Salt Reactor Campaign, DOE-NE-5.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2020

Mechanistic source term development for liquid fueled MSRs - Model Development Update

This report provides results from a critical literature review on the development of a mechanistic source term model (MST) for liquid fueled molten salt reactors (MSRs). It is submitted in fulfillment of milestone M4AT-20AN040601075 in the Advanced Reactor Technologies Molten Salt Reactors Campaign work package AT-20AN04060107.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2025

Benchtop-Scale High Temperature Molten Salt Electrochemical Reactors: Experimental Setup and Considerations

Molten salt electrochemical reduction (MSER) is the dominant production method for aluminum and titanium, and emerging technologies for producing other commodity metals with these highly electrified techniques have demonstrated promising results. However, the scale up of MSER of materials such as iron and silicon are limited by the challenging issues of materials compatibility and impurity control. This work describes an experimental MSER setup using both chloride and carbonate salts. This setup is designed for operations outside of a glovebox, which is practical from an industrial perspective, but creates unique challenges. This work serves as a practical guide to discuss some key operational difficulties such as temperature control, air and humidity, material compatibility, developing strong electrical measurements and techniques, and safety.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

SAM Enhancements and Model Developments for Molten-Salt-Fueled Reactors

To support the development and utilization of the SAM code for molten-salt-fueled reactor (MSR) safety analysis and licensing, an effort was devoted to enhancing code capabilities and developing reference models for the MSR primary loop. A reference standard problem of a prototypical reactor design is foundational to NRC to verify the adequacy of computer codes and evaluation models for a specific reactor type. A thermo-fluid model of the Molten Salt Reactor Experiment (MSRE) has been developed. The MSRE primary loop model consists of a 2-D core region and external core components in 1-D or 0-D. Both the steady-state and a transient scenario are simulated. The porous medium model is utilized for both the molten salt fluid channels and the moderator matrix in the MSRE core. The use of the porous medium model for the MSRE core is verified with the higher-fidelity simulation results using 1-D representations of the fluid channels and 3-D modeling of core structures. To further enhance SAM multi-scale simulation capabilities for MSRs, a mass transport model is developed and implemented in SAM multi-dimension flow module for modeling of species transport such as delayed neutron precursors in MSRs.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2023

Reevaluating the Thermal-Spectrum Molten Salt Breeder Reactor Fuel Cycle in a Modern Context [Slides]

Thermal-Spectrum Molten-Salt Breeder Reactors (TS-MSBRs) can have highly advantageous characteristics. There is potential for excellent safety, actinide resource utilization, proliferation resistance, waste generation, and exergy characteristics. Realizing advantageous characteristics derives from a combination of proper design/engineering and inherent properties. Grossly unacceptable properties are possible with poor design choices. TS-MSBR designs and technologies remain immature. The United States has not had a focused TS-MSBR program in nearly 50 years. TS-MSBRs have progressed due to: (1) technology development in related areas (fusion, materials, instrumentation); (2) general, worldwide molten-salt reactor (MSR) development activities; (3) molten-salt property measurement and evaluation; and (4) safety evaluation methods and performance-based, technology neutral licensing.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

SAM Developments for MSR Modeling (FY21)

An advanced system analysis tool, SAM, is under development for advanced non-LWR reactor safety analysis, including molten salt reactors (MSR). To support the development and utilization of the SAM code for MSR safety analysis and licensing, continuous efforts have been devoted to enhancing code capabilities and updating reference models for the MSRs. This report documents the FY21 progress in SAM code development, capability enhancements, and reference model development to support transient safety analysis of MSRs, including code enhancements in reactor kinetics and reactivity feedback modeling for liquid fuel reactors, updates of the Molten Salt Reactor Experiment (MSRE) primary system model, developments and updates of the molten salt fast reactor (MSFR) model based on EVOL design, and implementation of a drift flux model for modeling gas transport in MSR systems.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

First-principles free energies by hybrid thermodynamic integration for phase equilibria and fission product solubility in molten salts

The overarching goal of this research project is quantitative microscopic modeling of phase diagrams and solubility of actinides and lanthanide-fission products in molten salts for molten salt reactors. Application of molten salts as coolants and liquid fuels for next-generation reactors requires quantitative understanding of phase diagrams, equations of state and transport properties of binary and ternary molten salt mixtures, as well as solubility of fuel, fission products and reactor-wall corrosion products, but these remain beyond the reach of current first-principles computational techniques. We will address this fundamental capability gap using a novel hybrid framework for thermodynamic integration to directly predict absolute free energies of solid and molten salts at any specified conditions of composition, temperature and pressure. This framework will combine a hierarchy of first-principles, molecular dynamics and continuum techniques to deliver first-principles-level accuracy at a fraction of the computational cost of conventional ab initio molecular dynamics approaches. In particular, this technique is expected to provide first-principles accuracy, while off-loading most of the computational work on much less expensive classical molecular dynamics and continuum techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Mechanistic Source Term Considerations for Advanced Non-LWRs

This report is a functional review of the radionuclide containment strategies of fluoride-salt-cooled high temperature reactor (FHR), molten salt reactor (IVISR) and high temperature gas reactor (HTGR) systems. This analysis serves as a starting point for further, more in-depth analyses geared towards identifying phenomenological gaps that still exist, preventing the creation of a mechanistic source term for these reactor types. As background information to this review, an overview of how a mechanistic source term is created and used for consequence assessment necessary for licensing is provided. How mechanistic source term is used within the LMP is also provided. Third, the characteristics of non-LWR mechanistic source terms are examined This report does not assess the viability of any software system for use with advanced reactor designs, but instead covers system function requirements. Future work within the Nuclear Energy Advanced Modeling and Simulations (NEAMS) program will address such gaps.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Mechanistic Source Term Considerations for Advanced Non-LWRs (Revision 1)

This report is a functional review of the radionuclide containment strategies of fluoride-salt-cooled high temperature reactor (FHR), molten salt reactor (MSR) and high temperature gas reactor (HTGR) systems. This analysis serves as a starting point for further, more in-depth analyses geared towards identifying phenomenological gaps that still exist, hindering the creation of a mechanistic source term for these reactor types. As background information to this review, an overview of how a mechanistic source term is created and used for consequence assessment necessary for licensing is provided. How a mechanistic source term is used within the Licensing Modernization Project (LMP) is also provided. Lastly, the characteristics of non-LWR mechanistic source terms are examined. This report does not assess the viability of any software system for use with advanced reactor designs, but instead covers system function requirements. Future work within the Nuclear Energy Advanced Modeling and Simulations (NEAMS) program will address such gaps. This document is an update of SAND 2020-6730. An additional chapter is included as well as edits to original content.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Mechanisms of Retention and Transport of Fission Products in Virgin and Irradiated Nuclear Graphite

To fulfill the design and licensing requirements for advanced reactors, the U.S. Department of Energy (DOE) is specifically interested in targeted research to quantify the mechanisms of fission product transport and retention in graphitic grades that will likely be used in next-generation very/high temperature reactors, fluoride salt-cooled high temperature reactors and molten salt reactors. We have examined an integrated experimental-computational approach to determine the diffusivities of selected fission products – ruthenium (Ru) and silver (Ag) in five nuclear graphite grades – POCO AXF-5Q, POCO ZXF-5Q, PCEA, IG110, and NBG-18. Experimental investigation for diffusion of other fission products (iodine, cesium, and krypton) in graphite could not be carried out due to extreme evaporation due to high vapor pressure, despite several attempts incorporating various experimental schemes. Experimental investigation with irradiated graphite could not be carried out because necessary approval to transport irradiated graphite could not be obtained due to procedural reasons at ORNL and national policy change in UK. An effort was made to “produce” by ion sputtering, but it was discontinued because the outcome did not adequately represent irradiated graphite. Thin film and “cup-and-cap” methods were employed to deposit fission products, diffusion annealed were carried out in an argon atmosphere, and concentration profiles were determined by dynamic secondary ion mass spectroscopy depth profiling technique. Regardless of graphite type, anomalous diffusion behavior of Ru (i.e., lower than expected based on Arrhenius temperature dependence) at an intermediate temperature, around 600 to 700 °C, was observed. Diffusion behavior of silver on the other hand agreed well to the Arrhenius temperature dependence although the excessive evaporation of silver hampered the accurate determination of diffusivities at temperature higher than 900 °C. In general, silver was observed to diffuse faster than Ru in the temperature range compared from 500 to 900 °C, had consistently had higher pre-exponential factor corresponding to higher jump frequency. To understand the abnormal diffusional behavior of Ru in graphite in intermediate temperature range, a detailed microstructural analysis was carried out. Clustering of Ru into particles on the surface of graphite was observed around 700 °C corresponding to de-wetting and spheroidization. This change would influence the boundary condition of diffusion, although features of clustering was much smaller (<1 mm) than the SIMS raster size (120 x 120 mm). Raman spectroscopy also demonstrated that Raman peak intensity for Ru decreased significantly for samples annealed higher than 700 °C and presence of Ru in graphite altered the crystallinity of graphite. To further elucidate the abnormal diffusion behavior observed in intermediate temperature investigated, the vibrational properties of graphene, bilayer graphene and Kr atoms in bilayer graphene were investigated with molecular dynamics. Krypton, which is a fission product, was introduced between a bilayer graphene system to evaluate (i) whether the phonon dispersion curves change with high temperature in bilayer graphene (ii) whether the addition of Kr atoms between the bilayer introduces any significant change in the vibrational properties, and (iii) whether any change in the vibrational properties can be correlated to the diffusive behavior of Kr atoms. The results show that the Kr atoms indeed exhibit an anomalous diffusive behavior at 550°C. Phonon analysis shows that a few phonon frequencies are enhanced as much as 20 to 30 % with the addition of just 0.2 at.% Kr. So, this may explain the unexpected self-diffusivity of fission products.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Radiation Stability of MOF Engineered Particles

Pacific Northwest National Laboratory (PNNL), in collaboration with Flibe Energy, demonstrated the fabrication of metal organic frameworks (MOFs) into engineered beads to manage off-gases released from advanced reactors, including molten salt reactors. Based on the commercial availability and easy to synthesis at scale, PNNL down-selected two MOF sorbents known as CuBTC and UiO-67. The sorbents were synthesized, characterized, and fabricated into mechanically robust engineered beads (composites) using wet granulation method using polymer as a binder. Further, MOF powders and and mechanically robust composites were exposed to gamma radiation using Co-60 source and characterized irradiated MOFs to demonstrate the structural stability. Among the two MOF sorbents identified, the CuBTC MOF was shown to be very promising for noble gas management at low temperature (193 K) compared to UiO-67 MOF. The high adsorption capacity of the synthesized composites was correlated to the high surface area and pore volume of the CuBTC MOF. Both MOFs retain structural integrity and long-range order even after exposure to 1000 kGy of radiation.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2022

Real-Time Inventory Change Detection for the Protactinium Decay Inventory of the Molten Salt Breeder Reactor

This work presents a novel monitoring method for detecting material loss from the decay inventory of the molten salt breeder reactor (MSBR) by monitoring for changes to the system dynamics using an isotopic ratio. Here the isotopic masses in the decay inventory of a MSBR were simulated under several material loss scenarios. In each case, the ratio of 231 Pa to 233 Pa served as a sensitive and lasting indicator of material loss. This isotope ratio quickly decreased outside the normal range after a material loss, and the ratio remained depressed for several years after the loss. The dynamics of this ratio were driven by the periodic batch discard from the decay inventory every 220 days, which was specified in the MSBR design to periodically remove fission product buildup. For this method, isotopic ratios were found to be rapid and enduring indicators of inventory change if they comprise a pair with a short half-life (e.g., 233 Pa) and a long half-life (e.g., 231 Pa) relative to the effective half-life induced by the driving system process (e.g., the batch discard cycle). Using such an isotope pair enabled a method to monitor for changes to the effective half-life of the system and by extension changes to the system inputs and outputs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2021

Overview of Advanced Reactor Simulation Capabilities to Support Demonstrations

The Virtual Test Bed (VTB) was established to support the deployment of advanced reactors by facilitating the use of state-of-the-art modeling and simulation capabilities. These tools are able to solve previously prohibitive challenge problems in greater levels of fidelity and in a multi-physics framework. A VTB repository was recently set up to host models for a wide variety of reactor types and using a range of NEAMS-developed software. Table I summarizes the different capabilities already available in the repository and up-and-coming near/long term ones. The repository currently hosts models for a wide variety of reactor types, including High-Temperature Gas Cooled Reactors (HTGR), Sodium Fast Reactors (SFR), Fluoride salt cooled High-temperature Reactors (FHR), Molten Salt Reactors (MSR), and Heat-Pipe Microreactors (HP-MR). It should be noted that work is ongoing for all of the models and each example problem is at a different state of maturity.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2024

MSR Transient Simulation and MSRE Transient Benchmark with SAM and SPECTRA

In recent years, there has been renewed interest in molten salt reactors (MSRs) for their potential advantages compared to reactors that rely on solid fuel. In response to such interest, many methods and codes have been developed to capture the unique features of MSRs. Among them, SPECTRA and SAM are two system analysis codes that have been enhanced to include MSR-specific modeling capabilities, including delayed neutron precursor drift and modified point kinetics equations.This paper discusses the efforts taken to verify and validate these features. A standard MSR system test problem was developed to verify and demonstrate the capability of SPECTRA and SAM on the MSR transient simulation. Sixteen transients were simulated. Further, the results obtained from SPECTRA and SAM show good agreement. The Molten Salt Reactor Experiment transient experiments were reviewed and selected to validate the SPECTRA and SAM codes. The experiments included pump startup and coastdown tests at zero power, reactivity insertion tests at different power levels, frequency tests, and a natural convection test. The simulation results from SPECTRA and SAM show good agreement with the experimental data.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2022

Preconceptual Design of Irradiated Fuel Salt Management System

The National Reactor Innovation Center was established by the U.S. Department of Energy to accelerate the demonstration and deployment of advanced nuclear reactors. To meet this mission, the National Reactor Innovation Center has developed the Laboratory for Operations and Testing in the U.S. (LOTUS) to support the first fast-spectrum molten salt reactor demonstration. The goal of this research is to understand the system requirements that may be applied to a molten salt reactor experiment in the LOTUS test bed and to perform systems analyses and preconceptual development of a storage container for the management of the irradiated molten salt fuel. This study proposes a set of irradiated fuel salt management processes for the molten salt reactor, from defueling to storage or disposal. For that, the historic Molten Salt Reactor Experiment (MSRE) at Oak Ridge National Laboratory has served as a crucial source of data for a mock application. This paper proposes a potential geometry for storing irradiated fuel salt based on MSRE data and the Monte Carlo N-Particle radiation transport code. The geometry was analyzed for criticality safety under abnormal situations, such as water ingress and interaction between containers. Based on the determined configuration of the storage system, the decay heat produced from the irradiated fuel salts was calculated to provide a reasonable time scale of the dormancy period. Using the same geometry assumed above, the neutron and gamma dose rates from the irradiated fuel salt at the end of the dormancy period were estimated, which will be useful for understanding the handling and radiation protection requirements for handling the irradiated fuel salt. Lastly, a reactor in the LOTUS test bed could use chloride-based fuel as opposed to the fluoride-based fuel used in MSRE. Thus, a literature study provided data to understand the similarities and differences between the characteristics of fluoride- and chloride-based salts in terms of salt chemistry, material characteristics, postirradiation behavior, neutronics, thermal hydraulics, and heat removal. This study, together with the proposed irradiated fuel salt management processes, preliminary criticality calculations, decay heat, and dose rate estimates, provides a strong basis for future investigation into the management of irradiated fuel salts generated during molten salt reactor technology demonstrations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

U.S. MSR Development Programs & Supportive Efforts [Slides]

The presentation provides a summary of recent activities within the U.S. on molten salt reactors (MSRs). The presentation is intended for the Generation IV International Forum's MSR provisional system steering committee meeting in November 2023. The presentation includes U.S. government, industry, national laboratory, and university led activities.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2024

Assessment of Technical Information Needs and Considerations for Front-End Activities for Molten Salt Fuel Types

This report details an assessment of the hazards and safety impacts related to front-end operations of molten salt reactors (MSR) as well as an assessment of existing safety guidance. Publicly available information was evaluated to make recommendations to the U.S. Nuclear Regulatory Commission (NRC) for guidance development and information gathering needs. Five different MSR technologies were evaluated along with information from 1960’s about the Atomic Energy Commission programs for the Aircraft Reactor Experiment and Molten Salt Reactor Experiment. Primary areas of evaluation include fuel cycle facilities, transportation and at reactor fuel mixing operations up to reactor startup. In general, there was difficulty synthesizing publicly available information due to the early stage of the MSR development and proprietary information associated with the reactor technology companies analyzed. There are a few specific recommendations from this report. One overarching paradigm shift that the NRC needs to evaluate is the possibility of collocating fuel cycle facilities with operating MSRs. Although there is no specific prohibition to this in the NRC regulations, the collocation of the fuel cycle facilities with the operating MSR presents a novel approach compared to the light water reactor baseline. More guidance and research into thorium operations and regulation is needed. The hazards associated with the stability of stored fuel constituents need to be evaluated. Some reactor fuel cycles use beryllium, and its use and the associated hazards need further analysis. NRC-approved designs for transportation packages for shipping molten salt fuels and factory-built and fueled reactors are not available.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2023

Concept for an irradiation experiment to test a laser-induced breakdown spectroscopy off-gas sensor for molten salt systems

This paper focuses on laser-induced breakdown spectroscopy (LIBS) as an off-gas sensor and details a conceptual irradiation experiment to evaluate its performance in an environment that is more realistic of an operational molten salt reactor (MSR). MSRs are a promising advanced nuclear design that use high-temperature liquid salts as the coolant, fuel, or a combination of both. They will generate and subsequently evolve fission products into the reactor headspace during operation. These evolved fission products will necessitate an online off-gas system to treat the reactor cover gas before recycling it to the core. Such a system, especially during the early deployment phase, will benefit from online sensors to inform operators of the treatment system’s performance. Optical spectroscopy is well-suited to fit this task as it can be remotely deployed using fiber-optics and can detect most species at high frequencies. LIBS can detect nearly every element on the Periodic Table, stable or radioactive, making it an ideal candidate. The provided conceptual experiment discusses the facility requirements, salt capsule design, and detailed testing campaigns with corresponding simulated LIBS spectra.

47 OTHER INSTRUMENTATION↗