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  1. Novel Calibration Approach for Monitoring Aerosol Hydrogen Isotopes Using Laser-Induced Breakdown Spectroscopy for Molten Salt Reactor Off-Gas Streams

    Online monitoring is a key challenge for the continued development of molten salt reactor (MSR) technology. Laser-induced breakdown spectroscopy (LIBS) has previously been demonstrated to be a viable tool for monitoring aerosolized species and noble gases in real time, but the ability to discern varying isotopes in these streams has not yet been investigated for MSR applications. Tritium will form in MSRs from ternary fission and from (n,α)-reactions occurring in lithium-containing salts. This study compares three spectrometers of varying resolutions and types for measuring hydrogen isotope shifts in LIBS spectra of wetted filter paper. For each spectrometer, multivariate models weremore » built (i.e., principal component regression, partial least squares regression, and multivariate curve resolution) to quantify the isotope ratio. The top models were then modified and corrected to apply the models to aerosol samples with varying isotope ratios. This novel calibration strategy offers an 82% reduction in volume of the calibration samples needed and is a more viable pathway for calibrating deployable LIBS systems. Lastly, this calibration model was compared with an all-aerosol trained model for monitoring hydrogen isotopes during a real-time test where the protium/deuterium ratio, along with representative salt species (i.e., lithium, sodium, and potassium) were adjusted dynamically. Results of this test validated the predictive capabilities of the transferred model and highlighted the capabilities of LIBS for real-time monitoring of MSR effluent streams.« less
  2. Complex Structure of Molten FLiBe (2 Li F Be F 2 ) Examined by Experimental Neutron Scattering, X-Ray Scattering, and Deep-Neural-Network Based Molecular Dynamics

    The use of molten salts as coolants, fuels, and tritium breeding blankets in the next generation of fission and fusion nuclear reactors benefits from furthering the characterization of the molecular structure of molten halide salts, paving the way to predictive capability of the chemical and thermophysical properties of molten salts. Due to its neutronic, chemical, and thermochemical properties, 2LiF-BeF2 is a candidate molten salt for several fusion- and fission-reactor designs. We performed neutron and x-ray total-scattering measurements to determine the atomic structure of liquid 2LiF-BeF2. We also performed ab initio and neural-network molecular-dynamics simulations to predict the structure obtained bymore » neutron- and x-ray-diffraction experiments. The use of machine learning provides improvements to the efficiency in predicting the structure at a longer length scales than is achievable with ab initio simulations at significantly lower computational expense while retaining near ab initio accuracy. We found that the NNMD simulations accurately predicted the $Be$$$${F}^{2-}_{4}$$ oligomer formations seen in the experimental first-structure-factor peak. Our combination of high-resolution measurements with large-scale molecular dynamics provided an avenue to explore and experimentally verify the intermediate-range ordering beyond the first-nearest neighbor that has posed too many experimental and computational challenges in previous works. With a deeper understanding of the salt structure and ion ordering, the evolution of salt chemistry over the lifetime of a reactor can be better predicted, which is crucial to the licensing and operation of advanced fission and fusion reactors that employ molten salts. To this end, this work will serve as a reference for future studies of salt structure and macroscopic properties with and without the addition of solutes.« less
  3. High-gradient magnetic separation of colloidal uranium oxide particles from soil components in aqueous suspensions

    The separation of uranium oxide (UO2) particles from soil-surrogate particles in aqueous suspensions was achieved using filtration enhanced by a magnetic field. Enhanced attraction of paramagnetic UO2 colloids to a ferromagnetic stainless-steel filter placed in a strong magnetic field arises because of the positive magnetic susceptibility of the particles and the high-gradient field generated near ferromagnetic fibers. Enhanced uptake of smaller particles over larger ones occurs through Brownian motion that promotes the collision of particles with the ferromagnetic fibers of the filter. Hence, this work focused on UO2 particles in the colloidal size range. Experiments used a water-cooled electromagnet andmore » an array of permanent magnets. Chemical analysis showed that the magnetic field increased the capture efficiency of uranium particles from a range of 27–53% with the magnet off up to 98% with the magnet on after a single pass of the suspension through the filter. Further, the recovery of the UO2 particles from the filter, however, was more difficult to achieve. Small amounts of UO2, together with significant amounts of background SiO2 particles, were removed from the filter during a first flush with the magnetic field on. A much larger recovery of UO2 was not observed until a second out-of-field flush was performed, which also released some SiO2. The degree to which particle separation was enhanced through the use of multi-stage filtration compared to single pass-through filtration was also examined. A design was suggested that could be used to optimize the separation efficiency for a continuous process.« less
  4. Establishing Isotopic Measurement Capabilities using Laser-Induced Breakdown Spectroscopy for the Molten Salt Reactor Campaign

    Proof-of-principle H isotope ratios of aqueous aerosol systems and liquid droplets on filter paper have been measured using laser-induced breakdown spectroscopy (LIBS) with root mean square error of prediction values down to 1.9%. Molten salt reactors (MSRs) will consist of a complex chemical and radiological system consistently producing new fission products as the reactor operates. Some of these fission products and/or their daughter species will leave the salt in the reactor off-gas. Monitoring the composition of the off-gas, as well as the salt itself, is important for monitoring reactor performance, including burnup, corrosion, and the concentration of impurities. Tritium ismore » of concern for MSRs because it will be produced from the irradiation of key salt constituents, including Li and Be. LIBS offers an avenue for in situ salt and off-gas monitoring by firing a laser onto or into the sample stream to generate a plasma. The plasma light can be monitored to measure an elemental fingerprint of the sample. Extending this analysis to include isotopic ratios offers a critical expansion of the in situ monitoring capabilities being developed. This study demonstrates the expansion of Oak Ridge National Laboratory’s LIBS capabilities to monitor isotopes and shows how simple calibrations may provide rapid semiquantitative models.« less
  5. Technologist in Residence for Advanced Manufacturing and Materials in Unconventional Oil and Gas Equipment and Infrastructure

    The DOE Technologist in Residence (TIR) program pairs a senior technical staff member from a National Laboratory (Lab Technologist), and a senior technical staff member(s) from a clean energy manufacturing company or consortium of companies (Industry Technologist). Each technologist may represent single or multiple national laboratories, or single or multiple companies. These pairs of Lab and industry technologists work together for a period of 18 to 24 months to accomplish several goals: 1) Identify the participating company’s (or companies’) technical priorities and challenges, and the resources and capabilities in DOE’s National Laboratories that may be highly suitable to address them;more » 2) Propose collaborative R&D efforts to develop science-based solutions to the company’s (or companies’) most strategic scientific, technological, and business issues; and 3) Develop a general framework agreement and begin developing specific scopes of work for the proposed collaborative R&D efforts. The proposed R&D will then take place outside of the program and will not use TIR program funds. Oak Ridge National Laboratory (ORNL) and Pioneer Natural Resources were awarded a TIR project by DOE in late 2016 and the CRADA component of the project was initiated in 2017. This report describes work performed under the CRADA agreement between 2017 and 2020.« less
  6. Design of Instrumentation for Noble Gas Transport in LSTL Needed for Model Development

    Development of molten salt reactors (MSRs) requires consideration of several physical phenomena that are different from the light water reactor (LWR) experience. While small-scale tests have been performed to understand the behavior of molten salts, the scale-up to larger experiments is an important step in the development of MSR designs. These small-scale experiments have given information on the thermodynamic state of the heat transport fluid and its constituents, thermophysical properties, convective flow, and corrosion. As detailed models have been developed, using these models to simulate larger scale experiments must incorporate physics that becomes important during scale-up, temperature inhomogeneities, complex flowmore » behavior, and two-phase flow. The purpose of the work package has been to link experimental and modeling efforts in the support of licensing development to design and evaluate technologies to mitigate radionuclide release from MSRs. There were two main activities in this work package—one investigating fission product transport into the cover gas and the other on fission gas transport in the molten salt.« less
  7. Commercially available Hydrogen Detection Systems for Corrosive, Oxygen-free Gas Streams: A Technical Summary

    The growing use of hydrogen gas across energy, transportation, and chemical applications necessitates better hydrogen sensors and detectors. Few sensors exist for quantifying hydrogen gas in a corrosive, oxygen-free gas stream due to the challenging nature of the sampling environment and current technological status. Handheld, economic options include palladium-based, metal oxide, catalytic bead, and electrochemical sensors. More permanent and costly options include electrochemical sensors, thermal gas analyzers, mass spectrometers, gas chromatographs, and Raman spectrometers. In this technical report, a short review of current technology, along with the associated commercially available products, is provided. Raman spectroscopy is recommended as an idealmore » technology for on-line detection of hydrogen at low concentrations in a corrosive, oxygen-free gas stream.« less
  8. Technology Development Roadmap for Volatile Radionuclide Capture and Immobilization

    An “Off-Gas and Waste Forms Strategy Workshop” was held in Washington, D.C. on January 31, and February 1, 2023, to review the current state of the art (baseline) technologies for capturing and immobilizing these volatile radionuclides in waste forms (WFs). The discussions in that workshop were used to develop a roadmap for future research and development to mature technologies that are presently not ready for use in a commercial reprocessing facility and develop and demonstrate technologies that provide more safety, more simplicity, or lower costs compared to the current baseline.
  9. Scaled up Process Report – Apparatus and Model

    Advanced voloxidation with NO2 is a proposed process for used nuclear fuel head-end reprocessing scheme that converts UO2 to higher oxides, and it also converts partitioning volatile fission products into the gas phase, thus facilitating fuel dissolution and actinide recovery. NO2 voloxidation is being studied on small batches of UO2 Simfuel, but the real test of process feasibility will be when it is scaled up to work with >100 g of irradiated material. This report discusses the aspects of scale-up that must be considered for NO2 voloxidation, including development of a stirred reactor to promote agitation of the mixture duringmore » processing, online process monitoring, and automation controls. Brief details on parallel efforts are also provided in this report, including (a) demonstration of iodine release from Simfuel made by Spark Plasma Sintering, and (b) development of an order-of-magnitude scale-up to react 100 g of UO2 Simfuel in a metal reactor.« less
  10. A Review of Advanced Test Reactor Fuel and Assessment of Its Compatibility with the ZIRCEX Chlorination Process

    Advanced Test Reactor (ATR) fuel has been identified as a resource for high-assay low-enriched uranium (HALEU) production. A survey was performed on the published literature describing ATR fuel. The geometry of the fuel is complex; different parts of the fuel compact experience differing neutron flux and burnup. The literature is sparse, and access is controlled. Therefore, fundamental studies of fuel reprocessing must use a model fuel that represents the main chemical and structural features. Advanced chlorination, or chlorination with sulfur-chlorine bearing reagents is being investigated as way to separate the fuel from metal matrix alloys. A UAlx alloy will bemore » fabricated with x = 3, 4, and 5. The potential chlorination of individual UAlx intermetallics will be assessed in the advanced chlorination process of Al-8001 and Al-6061 as well as a representative mixture. Initial studies will track the alloying elements of the Al, which are Si, Fe, Cu, Mn, Mg, Cr, Zn, and Ti, in addition to the U itself. Further studies will include fission product simulants. Because advanced chlorination solvents include sulfur, the chemistry of sulfur with major and minor constituents will also be investigated. The experimental work accompanied by neutronic calculations will allow the assessment of the feasibility of advanced chlorination to separate aluminum from uranium. If bench-scale testing appears promising, then small-scale tests in shielded facilities with irradiated cladding, lightly irradiated fuel, and spent nuclear fuel are recommended to track the complete inventory of fissile actinides, fission product impurities, and reagent solids and liquids.« less
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