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Depletion-driven thermochemistry of molten salt reactors: review, method, and analysis

Molten salt reactors (MSRs) are innovative advanced nuclear reactors that utilize nuclear fuel by dissolving it in a high-temperature liquid salt. This unique feature differentiates MSRs from other types of reactors and allows for enhanced safety and economic performance. The liquid fuel also entails several multiphysics effects that can complicate reactor design and operation. One primary effect termed here as depletion-driven thermochemistry is a driving force in altering the multiphysics behavior of the reactor. Essentially, depletion-driven thermochemistry is the effect that fuel depletion has on changing the chemical redox potential of the fuel salt over time. As the fuel is consumed, the redox potential shifts toward a more oxidizing state. Without active control, the changing chemistry due to depletion increases corrosion thereby limiting reactor component lifetimes. Additionally, the changing redox potential of the fuel salt alters the vapor pressures of chemical species dissolved in the fuel salt. Changing vapor pressures of species in the fuel salt is an important parameter to understand when off-gassing volatile species during normal reactor operation, and for source term characterization during accident scenario transients. The present work represents a fundamental step toward modeling and coupling the driving physics (i.e., neutronics and chemistry) involved in altering the redox potential in an MSR. Here, the neutronic code Griffin models the depletion of the fuel-salt system, while the chemical equilibrium code Thermochimica calculates the thermochemical state of the isotopic inventory, using the Molten Salt Thermodynamic Database - Thermochemical (MSTDB-TC). These two codes are tightly coupled to predict the impact of fuel depletion in altering the chemistry in MSR systems. Redox potential control methods are discussed and can be modeled using this multiphysics approach. The vapor pressures of chemical species that could be extracted to an off-gas system, as determined by the reactor’s thermochemical state, are examined. The neutronics-chemistry coupling developed in this work is expected to have potential application for analyzing corrosion, source term evolution, and material safeguards in MSR systems. Lastly, suggestions for areas of further improvements of the models to expand these capabilities by incorporating other coupled physics effects is provided.

Walker, Samuel A.↗

Improvement and Verification of Online Cross Section Generation Capability of Griffin for TRISO-fueled Reactors

Griffin, a MOOSE-based reactor multiphysics code jointly developed by Idaho National Laboratory and Argonne National Laboratory under the DOE Office of Nuclear Energy’s NEAMS program, has pursued the development of an online multigroup cross section generation capability for a few years to enable high-fidelity, problem-dependent neutronics analyses of advanced thermal reactors. Recent advancements in Griffin’s online multigroup cross section generation capability have significantly improved the accuracy, robustness, and efficiency of self-shielding calculations for both prismatic and pebble-bed TRISO-fueled reactor applications. Key developments include a unified fuel self-shielding method applicable to both TRISO and annular compact/spherical shell fuel zone geometries; an advanced Dancoff Category-based Equivalence Theory using a bell function for non-fuel resonance treatment, achieving more than an order-of-magnitude speedup compared to the Tone method; an on-the-fly multigroup equivalence approach to mitigate group condensation errors; and a streaming correction method for pebble-bed homogenization. A proof-of-concept demonstration of on-the-fly group condensation with consistent P0 transport correction was also achieved. The method reproduced direct fine-group solutions with excellent accuracy (eigenvalue errors within 10 pcm and pin-power differences within 0.5%), but due to performance limitations of the current fixed-source solver, improvements to solver efficiency will be addressed in future work. Verification tests were performed on graphite-moderated TRISO-fueled two-dimensional core benchmark problems representing gas-cooled microreactors, heat pipe-cooled microreactors, gas-cooled pebble-bed reactors, and fluoride salt-cooled high-temperature reactors. Across all cases, Griffin showed excellent agreement with Serpent2 continuous energy Monte Carlo solutions: eigenvalue errors within 200 pcm, pin-power root-mean-square errors within 2%, and control rod and drum worth errors less than 2%. It should be noted that, for the benchmark problem, cross section generation contributed less than 3% of the total simulation times. These results demonstrate that Griffin’s online cross section generation capability delivers accurate and efficient reactor physics solutions across a wide spectrum of TRISO-fueled advanced reactor designs. With further improvements to the fine-group fixed-source solver and planned extensions to depletion, transients, and coupled neutron–gamma transport, Griffin will be well-positioned to become a powerful and comprehensive tool for advanced reactor analysis.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Development of the MCNP-ORIGEN activation automation tool

This paper introduces the MCNP-ORIGEN activation automation tool for streamlining the calculation of experiment source terms. This tool couples the Monte-Carlo radiation-transport solver, MCNP to the depletion tool, ORIGEN-S. To showcase its current capabilities, this paper presents an activation analysis exercise, which is conducted with Serpent, and the results are com- pared. The experiment consists in a 90%-enriched uranium sphere surrounded by light water. A non-fissile cylinder is placed in the water, representing an irradiation experiment. We conducted simulations for 2 different cylinder materials: iron and cobalt at two different temperatures: 300 K and 900 K. The exercise consists of an irradiation of 50 days at a constant power of 5 MW, followed by a decay of 50 days. These studies highlight the discrepancies between how the different tools handle nuclear data. Finally, the results underscore multiple areas of possible improvement.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

MHD-240 Neutron Detection Efficiency and Sensitivity Calibration

The neutron detection efficiency of the MHD-240 scintillation detector was measured at Ohio University Edwards Accelerator Laboratory. Pulsed broad-spectrum sources from the 27 Al(d,n) and 9 Be(d,n) reactions were used to produce the neutrons. The neutron time-of-flight technique was used to make an energy-differential efficiency measurement. The measurements were made in a low rate pulse mode. The pulse height distribution was also recorded, and the data were used to derive a neutron sensitivity that would be applicable in a high rate environment such as a critical assembly where the detector would be expected to operate in a current mode.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Development of a rapid-transit system for precision nuclear physics measurements

A Rapid Belt-driven Irradiated Target Transfer System, named RABITTS, was developed for use at the Triangle Universities Nuclear Laboratory. This system allows for cyclic activation with neutron or photon beams, and measurement of reaction products using γ-ray spectroscopy. Both a 1 meter and 10 meter transfer system have been developed with transit times as low as 0.4 and 1.0 seconds, respectively. The systems are deployed at the tandem accelerator laboratory for use with monoenergetic neutron beams, and at the High-Intensity γ-ray Source facility for activation using photon beams. A detailed characterization of the systems’ performance and sensitivity is presented. In order to produce the highest accuracy cross-section data, a model for calculating corrections to cyclic activation with variable beam flux is developed and presented. We have commissioned these systems by measuring 197m Au, where we report a measured half-life of 7.73 ± 0.05 s and a 197 Au(n, n') 197m Au isomer production cross of 628 ± 28 mb at neutron energy E n = 2.0 MeV. In addition, we measured 90m Zr, where we report a measured half-life of 799.7 ± 8.0 ms and a 90 Zr(n, n') 90m Zr isomer production cross of 180 ± 12 mb at E n = 4.6 MeV. Furthermore, these measured half-lives are in excellent agreement with the evaluated values and the cross-section measurements are performed at previously unmeasured incident neutron energies.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Extreme matter meets extreme gravity: Ultraheavy neutron stars with phase transitions

The speed of sound of the matter within neutron stars may contain nonsmooth structure related to first- or higher-order phase transitions. Here we investigate what are the observable consequences of structure in the speed of sound, such as bumps, spikes, step functions, plateaus, and kinks. One of the main consequences is the possibility of ultraheavy neutron stars (with masses larger than 2.5 solar masses), mass twins in heavy (with masses larger than 2 solar masses) and ultraheavy neutron stars. These stars pass all observational and theoretical constraints, including those imposed by recent LIGO/Virgo gravitational-wave observations and NICER x-ray observations. Here we thoroughly investigate other consequences of this structure in the speed of sound to develop an understanding of how nonsmooth features affect astrophysical observables, such as stellar radii, tidal deformability, moment of inertia, and Love number. Our results have important implications for future gravitational wave and x-ray observations of neutron stars and their impact in nuclear astrophysics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

The study of C-13(a, n)O-16 reactions in the Majorana Demonstrator calibration data

Neutron captures and delayed decays of reaction products are common sources of backgrounds in ultra-rare event searches. In this work, we studied 13C(a, n)1640 O reactions induced by a-particles emitted within the calibration sources of the Majorana Demonstrator. These sources are thorium-based calibration standards enclosed in carbon-rich materials. The reaction rate was estimated by using the 6129 keV ?-rays emitted from the excited 1643 O states that are populated when the incoming a-particles have enough energy. Thanks to the excellent energy performance of the Demonstrator’s germanium detectors, these characteristic photons can be clearly observed in the calibration data. Facilitated by Geant4 simulations, a comparison between the observed 6129 keV photon rates and predictions by a TALYS-based software was performed. The measurements and predictions were found to be consistent with each other, albeit with large statistical uncertainties. This agreement provides supports for further background predictions for (a, n)-reactions in future double-beta decay search efforts.

6 ≤ A ≤ 19↗

Chapter 10.02 - Neutron Scattering Studies of Materials for Hydrogen Storage

Hydrogen storage presents a significant barrier to the widespread adaptation of hydrogen as an energy source in mobile and stationary applications. The development of new candidate hydrogen storage materials is therefore an outstanding goal in the field of inorganic chemistry. Neutron scattering techniques - including diffraction, inelastic, and quasielastic scattering - are integral in investigating these materials. Here, we review some of the key studies of candidate hydrogen storage materials which have employed neutron scattering techniques. We begin with a brief discussion of hydrogen's current position in the global energy landscape. Next, we provide a brief description of the theory and practical aspects of the neutron scattering techniques germane to the study of hydrogen storage. Then we enumerate the neutron scattering studies of candidate hydrogen storage materials, including metal hydrides, chemical hydrides, and porous compounds. We focus on the studies which helped develop our understanding of hydrogen storage by revealing the underlying fundamental physics and chemistry of hydrogen sorption in these systems. Finally, we provide an outlook to the future of hydrogen storage research.

chemical hydrides↗

Proto-neutron star convection and the neutrino-driven wind: implications for the r-process

The neutrino-driven wind from proto-neutron stars is a proposed site for r-process nucleosynthesis, although most previous work has found that a wind heated only by neutrinos cannot produce the third r-process peak. However, several groups have noted that introducing a secondary heating source within the wind can change the hydrodynamic conditions sufficiently for a strong r-process to proceed. One possible secondary heating source is gravito-acoustic waves, generated by convection inside the proto-neutron star. As these waves propagate into the wind, they can both accelerate the wind and shock and deposit energy into the wind. Additionally, the acceleration of the wind by these waves can reduce the total number of neutrino captures and thereby reduce the final electron fraction of the wind. In neutron rich conditions, all of these effects can make conditions more favourable for r-process nucleosynthesis. Here, we present a systematic investigation of the impact of these convection-generated gravito-acoustic waves within the wind on potential nucleosynthesis. We find that wave effects in the wind can generate conditions favourable for a strong r-process, even when the energy flux in the waves is a factor of 10 –4 smaller than the total neutrino energy flux and the wind is marginally neutron rich. Nevertheless, this depends strongly on the radius at which the waves become non-linear and form shocks. We also find that both entropy production after shock formation and the acceleration of the wind due to stresses produced by the waves prior to shock formation impact the structure and nucleosynthesis of these winds.

79 ASTRONOMY AND ASTROPHYSICS↗

Neutron Star Equation of State in Light of GW190814

The observation of gravitational waves from an asymmetric binary opens the possibility for heavy neutron stars, but these pose challenges to models of the neutron star equation of state. Here, we construct heavy neutron stars by introducing nontrivial structure in the speed of sound sourced by deconfined QCD matter, which cannot be well recovered by spectral representations. Their moment of inertia, Love number, and quadrupole moment are very small, so a tenfold increase in sensitivity may be needed to test this possibility with gravitational waves, which is feasible with third generation detectors.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Total neutron cross-section measurement on CH with a novel 3D-projection scintillator detector

In order to extract neutrino oscillation parameters, long-baseline neutrino oscillation experiments rely on detailed models of neutrino interactions with nuclei. These models constitute an important source of systematic uncertainty, partially because detectors to date have been blind to final state neutrons. Three-dimensional projection scintillator trackers comprise components of the near detectors of the next generation long-baseline neutrino experiments. Due to the good timing resolution and fine granularity, this technology is capable of measuring neutron kinetic energy in neutrino interactions on an event-by-event basis and will provide valuable data for refining neutrino interaction models and ways to reconstruct neutrino energy. Two prototypes have been exposed to the neutron beamline at Los Alamos National Laboratory (LANL) in both 2019 and 2020, with neutron energies between 0 and 800 MeV. In order to demonstrate the capability of neutron detection, the total neutron-scintillator cross section as a function of neutron energy is measured and compared to external measurements. The measured total neutron cross section in scintillator between 98 and 688 MeV is 0.36 ± 0.05 barn.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Algorithm-Driven Advances for Scientific CT Instruments: From model-based to deep learning-based approaches

Multiscale 3D characterization is widely used by materials scientists to further their understanding of the relationships between microscopic structure and macroscopic function. Scientific computed tomography (SCT) instruments are one of the most popular choices for 3D nondestructive characterization of materials at length scales ranging from the angstrom scale to the micron scale. These instruments typically have a source of radiation (such as electrons, X-rays, or neutrons) that interacts with the sample to be studied and a detector assembly to capture the result of this interaction (see Figure 1 ). A collection of such high-resolution measurements is made by reorienting the sample, which is mounted on a specially designed stage/holder after which reconstruction algorithms are used to produce the final 3D volume of interest. The specific choice of which instrument to use depends on the desired resolution and properties of the materials being imaged. Additionally, the end goal of SCT scans includes determining the morphology, chemical composition, or dynamic behavior of materials when subjected to external stimuli. In summary, SCT instruments are powerful tools that enable 3D characterization across multiple length scales and play a critical role in furthering the understanding of the structure–function relationships of different materials.

42 ENGINEERING↗

Gamma and Neutron Measurement and Modeling of Irradiated TRISO Fuel

Given the unique characteristics of the PBR fuel cycle, both gamma and neutron measurements are expected to play important roles in performing and maintaining nuclear material control and accounting for spent pebbles to safeguard the fuel cycle. Given the lack of irradiated pebbles in the US, a variety of irradiated TRISO fuel samples with wide ranges of burnups and cooling times available at ORNL were used in this work. A large number of gamma and neutron measurements have been performed on these samples to collect data to test the various detectors and to benchmark the computer models to simulate the depletion and decay of the fuel and the measurements themselves. Two neutron detectors, including a custom-made detector and the Very High-Performance Neutron Multiplicity Counting, were used to measure the neutrons emitted by these TRISO samples. Three gamma spectrometry detectors, including an HPGe and the M400 CZT detector, were used to measure gamma-ray emissions from these samples. The M400 was recently adopted by the IAEA for fresh uranium measurements, but it was tested for spent fuel measurements prior to this project. Detailed MCNP models were developed to simulate these neutron and gamma measurements. Some GADRAS models were also developed to cross check the MCNP models for the gamma measurements. It was found challenging to perform neutron measurements in the hot cell due to the high background counts. Close agreements were observed between the simulated and measured neutron count rates in both detectors’ measurements of californium calibration sources. Both the HPGe and M400 detectors were able to measure the 604 and 662 keV peaks from these samples, which are the two most important peaks used to infer fuel burnup. Although the M400 detector did not have nearly good energy resolution and did not detect some of the minor peaks as the HPGe detector, it was found to be capable of handling significantly higher dose rates than HPGe. Given the complexities in the TRISO samples (e.g., different samples sizes) and uncertainties in the alignments between the detector and the TRISO fuel inside the containers, large scatters were found between the peak area rates and the samples’ burnups. However, the 604/662 peak ratios were found to trend well with the samples’ burnups among most samples in both measured and simulated results.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Impact of Source Geometry on Detector Response Matrix Efficiency: Simulations of the PFUNS-MUSiC Experiments

This work looks at two different bare highly enriched uranium (HEU) systems, configuration one from Measurements of Uranium Subcritical and Critical (MUSiC) and Prompt Fission Uranium Neutron Spectrum (PFUNS) to see the effect geometry has on detector efficiency and the response matrix. The distance from the multiplying source, the medium between the source and detector, and the geometry of the source all play a part in the efficiency of the detector. These factors are especially important when performing spectrum unfolding. Spectrum unfolding is a process used to reconstruct a true spectrum from measured detector response data. It involves interpreting a set of measured values, such as a light signal from a scintillator, to recover the original neutron energy spectrum. This leads to the question, how much will the efficiency of a detector change when you measure a point source compared to an extended source? The distance and solid angle from the source to the detector may be different. It may only be a minuscule change, but in the spectrum unfolding process it can have a considerable effect on the unfolded spectrum

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nuclear data uncertainty propagation and modeling uncertainty impact evaluation in neutronics core simulation

Uncertainty analysis is a critical requirement in reactor simulation as it is used to quantify the reliability of best-estimate calculation. A comprehensive uncertainty analysis should characterize all sources of uncertainties in a computationally-feasible and scientifically-defendable manner. Here we employ a well-established reduced order modeling (ROM) based uncertainty quantification methodology to propagate uncertainties throughout neutronic calculations. ROM relies on recent advances in randomized data mining techniques applied to large data streams. In our proposed implementation, the nuclear data uncertainties are first propagated from multi-group level through lattice physics calculation to generate few-group parameter uncertainties, described using a vector of mean values and a covariance matrix. Employing an ROM-based compression of the covariance matrix, the few-group uncertainties are then propagated through downstream core simulation in a computationally efficient manner. This straightforward approach, albeit efficient as compared to brute force forward and/or adjoint-based methods, often employs a number of assumptions that have been unquestioned in the literature of neutronic uncertainty analysis. This manuscript argues that these assumptions could introduce another source of uncertainty referred to as modeling uncertainties, whose magnitude needs to be quantified in tandem with nuclear data uncertainties. Thus, our primary goal is to explore the interactions between these two uncertainty sources in order to assess whether modeling uncertainties have an impact on parameter uncertainties. To explore this endeavor, the impact of a number of modeling assumptions on core attributes uncertainties is quantified. The study employs a CANDU reactor model, with Serpent and NEWT as lattice physics solvers and NESTLE-C as core simulator. The modeling assumptions investigated include those related with the uncertainty propagation method employed, e.g., deterministic vs. stochastic, the few-group energy structure employed to represent the cross-sections, the resonance treatment in lattice physics calculation, the reference values for the cross-section, and the number of samples employed to render ROM compression. Results indicate that some of the modeling assumptions could have a non-negligible impact on the core responses propagated uncertainties, highlighting the need for a more comprehensive approach to combine parameter and modeling uncertainties.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Optimizing the spatial resolution and gamma discrimination of SiPM-based Anger cameras

SiPM Anger cameras have been designed for use as 2-dimensional thermal neutron detectors for scientific applications such as at single crystal diffraction instruments. These cameras utilize a neutron sensitive scintillator and an array of SiPM photosensors, separated by a light spreading glass. While this optics package is very effective at detecting and positioning neutrons, it is also sensitive to gamma rays, which are a source of unwanted noise. In this work, we underwent a search of scintillator and spreader glass thicknesses to determine the optimal combination for maximizing spatial resolution. Both experimental results and GEANT4 simulations are presented. Further, to address the issue of gamma ray detection, we have also designed and presented a multi-layer scintillator that reduces the amount of scintillation light produced via gamma-ray energy deposition, allowing for easier pulse-height discrimination. A sample of this geometry has been produced that results in a factor of 2 improvement over an equivalent thickness monolithic scintillator.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗