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MARVEL Reactor Fuel Performance Report

The Microreactor Applications Research Validation and EvaLuation (MARVEL) project is producing a high temperature liquid metal-cooled nuclear test bed at Idaho National Laboratory (INL) to ultimately improve the integration of microreactors to end-user applications. This ambitious effort seeks to design, authorize, construct, test, and operate the reactor within five years. In order to construct and operate the MARVEL reactor in a timely manner, the system will utilize materials and component designs which have already been used, qualified, or licensed from previous reactors. The MARVEL reactor will be located at the INL Transient Reactor Test (TREAT) facility in the north high-bay equipment pit and will use the existing 304 stainless steel-clad U-ZrH1.6 pin-type fuel system developed by General Atomics and purchased from TRIGA International. This fuel has been previously qualified under the United States Department of Energy’s (US DOE) Reduced Enrichment for Research and Test Reactors (RERTR) Program. Even though the regulator of the MARVEL reactor is the US DOE, the standards and overall approach recommended by the Nuclear Regulatory Commission is well-defined and utilized here. Following NUREG-1537 regulatory guidance, this report documents the authorization case for the MARVEL fuel system’s application to MARVEL and establishes stable and predictable fuel performance during the most thermophysically unfavorable conditions achievable in the MARVEL reactor. To that end, this report provides a comprehensive survey of the known thermophysical properties, performance, and quantitative relationships associated with the MARVEL reactor fuel element and uses this information to determine its mechanical integrity and risk of reaching unacceptable conditions during the most extreme accident scenarios predicted for the reactor using the most conservative assumptions available. The information contained herein is compiled from a combination of historical reports and peer reviewed scientific publication manuscripts. Known mechanisms under which the fuel is susceptible to failure are highlighted and compared to conditions that could exist in the MARVEL reactor during an unanticipated transient or accident scenario. The two scenarios considered for analysis in this report are (1) an unprotected loss of flow accident and (2) a hypothetical unprotected loss of coolant accident during the loss of flow accident. Preliminary 2D steady-state analyses herein indicate that both fuel-cladding chemical interactions and fuel-cladding mechanical interactions are negligible throughout the fuel’s operational cycle under both normal and high temperature accident scenario conditions. Although higher fidelity 3D time-dependent modeling and simulations are planned, the following may be concluded presently. The MARVEL fuel element maintains its geometric stability and structural integrity during the most extreme accident scenarios predicted for the MARVEL reactor. The hoop stress during the unprotected loss of flow accident reaches about -1.27 MPa; this negative stress indicates that it is compressive rather than tensile. The compressive stress is a result of the NaK pressure on the outside of the fuel element, caused by the restricted thermal expansion of the NaK coolant, exceeding the internal pressures generated inside of the fuel element. The hoop stress generated in the cladding during the unprotected loss of coolant accident reaches a maximum of about approximately 10 MPa, which is nearly an order of magnitude less than the predicted yield strength of the cladding under high-temperature accident scenario conditions. Calculations were compared with results from high performance computational simulations using BISON and are in very close agreement. A conservative MARVEL fuel meat peak temperature limit of 900 °C is recommended presently, which is about 180 °C higher than the peak fuel temperature predicted to occur during the most extreme accident. Based on the known properties and behavior of the MARVEL fuel element, the fuel successfully meets its design and safety requirements under normal and most extreme accident conditions with a large safety margin.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Study of Convection Heat Transfer in a Very High Temperature Reactor Flow Channel: Numerical and Experimental Results

Very High Temperature Reactors (VHTRs) are one of the Generation IV gas-cooled reactor models proposed for implementation in next generation nuclear power plants. A high temperature/pressure test facility for forced and natural circulation experiments has been constructed. This test facility consists of a single flow channel in a 2.7 m (9’) long graphite column equipped with four 2.3kW heaters. Extensive 3D numerical modeling provides a detailed analysis of the thermal-hydraulic behavior under steady-state, transient, and accident scenarios. In addition, forced/mixed convection experiments with air, nitrogen and helium were conducted for inlet Reynolds numbers from 500 to 70,000. Our numerical results were validated with forced convection data displaying maximum percentage errors under 15%, using commercial finite element package, COMSOL Multiphysics. Based on this agreement, important information can be extracted from the model, with regards to the modified radial velocity and property gas profiles. Our work also examines flow laminarization for a full range of Reynolds numbers including laminar, transition and turbulent flow under forced convection and its impact on heat transfer under various scenarios to examine the thermal-hydraulic phenomena that could occur during both normal operation and accident conditions.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

The Effect of Balconies on Ventilation Performance of Low-rise Buildings

Chand et al. conducted experiments in a low speed wind tunnel to study the effect of balconies on the ventilative force on low-rise buildings without openings. Our study intends to investigate indoor ventilation performance by examining mass flow rate and average velocity on the working plane using computational fluid dynamics, using their model. Simulations were validated against their experiments. The numerical results indicate that, for single-sided ventilation, the provision of balconies increases mass flow rate and reduces average velocity on the working plane in most rooms, but for cross ventilation, this provision has no significant effect under normally or obliquely incident wind conditions. After the addition of balconies, the worst ventilation circumstances on the windward side under single-sided ventilation conditions were found on the intermediate floor. Furthermore, the simulation results also showed that, in many cases, wind flows into and out of the rooms through the left or right side of the opening rather than through the bottom and top of the opening, especially in the case of buildings that are obliquely oriented to the air stream. Finally, this phenomenon demonstrates that predictions of single-sided ventilative force using data relating to the bottom and top parts of the opening are not accurate enough.

42 ENGINEERING↗

In-situ Condition Monitoring of Components in Small Modular Reactors Using Process and Electrical Signature Analysis. Final report, volume 1. Development of experimental flow control loop, data analysis and plant monitoring

The research and development under this project was focused on the following three major objectives: Objective 1: Identification of critical in-vessel SMR components for remote monitoring and development of their low-order dynamic models, along with a simulation model of an integral pressurized water reactor (iPWR). Objective 2: Development of an experimental flow control loop with motor-driven valves and pumps, incorporating data acquisition and on-line monitoring interface. Objective 3: Development of stationary and transient signal processing methods for electrical signatures, machinery vibration, and for characterizing process variables for equipment monitoring. This objective includes the development of a data analysis toolbox. The following is a summary of the technical accomplishments under this project: - A detailed literature review of various SMR types and electrical signature analysis of motor-driven systems was completed. A bibliography of literature is provided at the end of this report. Assistance was provided by ORNL in identifying some key references. - A review of literature on pump-motor modeling and digital signal processing methods was performed. - An existing flow control loop was upgraded with new instrumentation, data acquisition hardware and software. The upgrading of the experimental loop included the installation of a new submersible pump driven by a three-phase induction motor. All the sensors were calibrated before full-scale experimental runs were performed. - MATLAB-Simulink model of a three-phase induction motor and pump system was completed. The model was used to simulate normal operation and fault conditions in the motor-pump system, and to identify changes in the electrical signatures. - A simulation model of an integral PWR (iPWR) was updated and the MATLAB-Simulink model was validated for known transients. The pump-motor model was interfaced with the iPWR model for testing the impact of primary flow perturbations (upsets) on plant parameters and the pump electrical signatures. Additionally, the reactor simulation is being used to generate normal operation data and data with instrumentation faults and process anomalies. A frequency controller was interfaced with the motor power supply in order to vary the electrical supply frequency. The experimental flow control loop was used to generate operational data under varying motor performance characteristics. Coolant leakage events were simulated by varying the bypass loop flow rate. The accuracy of motor power calculation was improved by incorporating the power factor, computed from motor current and voltage in each phase of the induction motor.- A variety of experimental runs were made for steady-state and transient pump operating conditions. Process, vibration, and electrical signatures were measured using a submersible pump with variable supply frequency. High correlation was seen between motor current and pump discharge pressure signal; similar high correlation was exhibited between pump motor power and flow rate. Wide-band analysis indicated high coherence (in the frequency domain) between motor current and vibration signals. - Wide-band operational data from a PWR were acquired from AMS Corporation and used to develop time-series models, and to estimate signal spectrum and sensor time constant. All the data were from different pressure transmitters in the system, including primary and secondary loops. These signals were pre-processed using the wavelet transform for filtering both low-frequency and high-frequency bands. This technique of signal pre-processing provides minimum distortion of the data, and results in a more optimal estimation of time constants of plant sensors using time-series modeling techniques.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Turbulent Flow Effects on the Biological Performance of Hydro-Turbines

The hydro-turbine industry uses Computational Fluid Dynamics (CFD) tools to predict the flow conditions as part of the design process for new and rehabilitated turbine units. Typically the hydraulic design process uses steady-state simulations based on Reynolds-Averaged Navier-Stokes (RANS) formulations for turbulence modeling because these methods are computationally efficient and work well to predict averaged hydraulic performance, e.g. power output, efficiency, etc. However, in view of the increasing emphasis on environmental concerns, such as fish passage, the consideration of the biological performance of hydro-turbines is also required in addition to hydraulic performance. This leads to the need to assess whether more realistic simulations of the turbine hydraulic environment -those that resolve unsteady turbulent eddies not captured in steady-state RANS computations- are needed to better predict the occurrence and extent of extreme flow conditions that could be important in the evaluation of fish injury and mortality risks. In the present work, we conduct unsteady, eddy-resolving CFD simulations on a Kaplan hydro-turbine at a normal operational discharge. The goal is to quantify the impact of turbulence conditions on both the hydraulic and biological performance of the unit. In order to achieve a high resolution of the incoming turbulent flow, Detached Eddy Simulation (DES) turbulence model is used. These transient simulations are compared to RANS simulations to evaluate whether extreme hydraulic conditions are better captured with advanced eddy-resolving turbulence modeling techniques. The transient simulations of key quantities such as pressure and hydraulic shear flow that arise near the various components (e.g. wicket gates, stay vanes, runner blades) are then further analyzed to evaluate their impact on the statistics for the lowest absolute pressure (nadir pressures) and for the frequency of collisions that are known to cause mortal injury in fish passing through hydro-turbines.

42 ENGINEERING↗

Experimental Investigation of Hydraulic Fracturing and Stress Sensitivity of Fracture Permeability Under Changing Polyaxial Stress Conditions

Understanding and predicting fracture propagation and subsequent fluid flow characteristics is critical to geoenergy technologies that engineer and/or utilize favorable geological conditions to store or extract fluids from the subsurface. Fracture permeability decreases nonlinearly with increasing normal stress, but the relationship between shear displacement and fracture permeability is less well understood. We utilize the new Geo–Reservoir Experimental Analogue Technology (GREAT cell), which can apply polyaxial stress states and realistic reservoir temperatures and pressures to cylindrical samples and has the unique capability to alter both the magnitude and orientation of the radial stress field by increments of 11.25° during an experiment. We load synthetic analogue materials and real rock samples to stress conditions representative of 500–1,000 m depth, investigate the hydraulic stimulation process, and then conduct flow experiments while changing the fluid pressure and the orientation of the intermediate and minimum principal stresses. High–resolution circumferential strain measurements combined with fluid pressure data indicate fracture propagation can be both stable (no fluid pressure drop) and unstable (fluid pressure drop). The induced fractures exhibit both opening and shear displacements during their creation and/or during fluid flow with changing radial stress states. Flow tests during radial stress field rotation reveal that fracture normal effective stress has first–order control on fracture permeability but increasing fracture offset can lead to elevated permeabilities at maximum shear stress. Here, the results have implications for our conceptual understanding of fracture propagation as well as fluid flow and deformation around fractures.

58 GEOSCIENCES↗

Evolutionary sheath structure in magnetized collisionless plasma with electron inertia

A classical hydrodynamic model is methodologically formulated to see the equilibrium properties of a planar plasma sheath in two-component magnetized bounded plasma. It incorporates the weak but finite electron inertia instead of asymptotically inertialess electrons. The effects of the externally applied oblique (relative to the bulk plasma flow) magnetic field are judiciously accented. It is, for the sake of simplicity, assumed that the relevant physical parameters (plasma density, electrostatic potential, and flow velocity) vary only in a direction normal to the confining wall boundary. It is noticed for the first time that the derived Bohm condition for sheath formation is modified conjointly by the electron inertia, magnetic field, and field orientation. It is manifested that the electron inertia in the presence of plasma gyrokinetic effects slightly enhances the ion Mach threshold value (typically, M{sub i0} ≥ 1.139) toward the sheath entrance. This flow supercriticality is in contrast with the heuristic formalism (M{sub i0} ≥ 1) for the zero-inertia electrons. A numerical illustrative scheme on the parametric sheath features on diverse nontrivial apposite arguments is constructed alongside ameliorative scope.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Multiphysics Analysis of Li Cooled Divertor Substrate During Loss of Coolant Accident (LOCA)

In the ongoing study of potential designs for liquid metal (LM) plasma-facing components (PFCs), so-called “slow” and “fast” Li flow divertor concepts are under investigation. In the previous studies on design and analysis of the slow Li flow divertor and comparison with the fast Li flow divertor, the magnetohydrodynamics (MHD)/heat transfer effects of the Li flowing inside the substrate as a second coolant were comprehensively investigated under the normal steady-state operation conditions. Here, in the present study, the multiphysics analysis is extended to the unsteady abnormal divertor scenario where the Li layer on top of the substrate does not provide full coverage or even totally disappears for a certain period of time, so that the substrate becomes directly exposed to the incident high plasma heat flux. Such an unwanted event may happen regardless of the concept of the divertor and is worth detailed investigations, typically referred to as a loss of coolant accident (LOCA). To address this situation, a simplified scoping analysis is conducted first in 2-D, and then an integrated 3-D modeling is performed using a time-dependent multiphysics model in COMSOL Multiphysics that integrates LM MHD, heat transfer, and solid mechanics. The main goal is to evaluate conditions under which the major material limits, such as the maximum allowable temperature, stress, and displacement of the substrate, can still be met. It was shown that the maximum time over which the substrate of RAFM steel can retain structural integrity during the LOCA is around 0.2 ∼ 0.3 s. Any divertor concept that utilizes RAFM steel as a substrate material and liquid Li as a second coolant should take such a permitted time into consideration.

divertor↗

Analysis of Postulated Accident Scenarios for the Transformational Challenge Reactor

The Transformational Challenge Reactor (TCR) is a helium-cooled, yttrium-hydride-moderated reactor that was designed for the U.S. Department of Energy Office of Nuclear Energy. A key objective of the TCR was to employ advanced manufacturing techniques in a nuclear system and demonstrate their potential for revolutionizing the nuclear reactor design process. One purpose of the present work is to demonstrate the safety of the TCR under postulated accidents. Based on RELAP5-3D and COMSOL analyses, the TCR remained below all current safety limits and far below the expected failure limits for the core materials. Another purpose of this work is to provide useful insights and recommendations regarding the application of RELAP5-3D to gas-cooled or other advanced reactors. A novel approach was implemented for simultaneously modeling conduction and radiation in RELAP5-3D, which was found to provide reasonable predictions of radial core, vessel, and ex-vessel heat transfer during postulated events. A multicode approach was also applied, in which high-fidelity COMSOL calculations were used to tune the radial heat transfer parameters in RELAP5-3D. The tuned RELAP5-3D model demonstrated comparable peak temperature predictions as COMSOL, despite a coarse treatment of the core in RELAP5-3D consisting of only two lumped heat structures. This high-fidelity tuning approach enabled enhanced accuracy as well as minimal complexity within the RELAP5-3D model, even for complex fuel geometric designs as in the TCR. Finally, investigations were made into the potential for flow reversal during a pressurized loss-of-forced-flow event in the TCR. The TCR is designed with downward helium flow through the core during normal operation. The RELAP5-3D model predicted that this downward flow would persist, without flow reversal, up to several days after the circulator trip. This was attributed to natural circulation hysteresis effects as have been noted in similar thermofluidic systems. Although flow stagnation and eventual reversal did not lead to unsafe TCR conditions, interesting spatial effects were observed which may have safety relevance for other reactor system designs and coolant types that are designed for downward core flow during normal operation, warranting closer investigation of the flow reversal phenomenon.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

On the physics-based processes behind production-induced seismicity in natural gas fields

Induced seismicity due to natural gas production is observed at different sites worldwide. Common understanding states that the pressure drop caused by gas production leads to compaction, which affects the stress field in the reservoir and the surrounding rock formations and hence reactivates preexisting faults and induces earthquakes. We show that the multiphase fluid flow involved in natural gas extraction activities should be included. We use a fully coupled fluid flow and geomechanics simulator, which accounts for stress-dependent permeability and linear poroelasticity, to better determine the conditions leading to fault reactivation. In our model setup, gas is produced from a porous reservoir, divided into two compartments that are offset by a normal fault. Results show that fluid flow plays a major role in pore pressure and stress evolution within the fault. Fault strength is significantly reduced due to fluid flow into the fault zone from the neighboring reservoir compartment and other formations. We also analyze scenarios for minimizing seismicity after a period of production, such as (i) well shut-in and (ii) gas reinjection. In the case of well shut-in, a highly stressed fault zone can still be reactivated several decades after production has ceased, although on average the shut-in results in a reduction in seismicity. In the case of gas reinjection, fault reactivation can be avoided if gas is injected directly into the compartment under depletion. However, gas reinjection into a neighboring compartment does not stop the fault from being reactivated.

03 NATURAL GAS↗

Investigation of temperature dependent microstructure evolution of pure iron during friction stir welding using liquid CO2 rapid cooling

Highlights: • Microstructure evolution during the FSW of pure iron was investigated under low and high heat input conditions, respectively. • Rapid cooling, tool stop action, marker insert and short-time annealing were employed to clarify the microstructure evolution. • Continuous and discontinuous dynamic recrystallizations occur during the microstructure evolution under both the conditions. • Incomplete and complete recrystallized microstructures were developed severally under the low and high heat input conditions. • Grain growth occurs during the normal cooling stage but it is very limited under the low heat input condition. - Abstract: The microstructure evolution of pure iron during friction stir welding was reconstructed by an ingenious experimental design, in which the rapid cooling friction stir welding combined with the tool “stop action” technique and the subsequent short-time annealing were adopted to “freeze” the transient microstructure during the stirring and reproduce the normal cooling during conventional friction stir welding, respectively. The microstructure evolution during the stirring and normal cooling was investigated along the material flow path and in the annealed “frozen” weld zone by high-resolution electron-backscatter-diffraction technique. The results show that the continuous and discontinuous dynamic recrystallizations occur simultaneously at the severe deformation stage in front of the tool both under low and high heat input conditions. However, during the material flow, the microstructure evolution involves the plastic deformation, recrystallization, high angle boundaries migration and dynamic recovery under the low heat input condition, while in a dynamic balance of deformation, recrystallization and grain growth under the high heat input conditions. At the cooling stage, normal grain growth occurs both for the low and high heat input welding conditions, while it is very limited for the low heat input condition.

36 MATERIALS SCIENCE↗

Thermal Model Heat Rate Predictions of the AGR-5/6/7 Experiment

Several fuel and material irradiation experiments have been planned for the U.S. Department of Energy Advanced Gas Reactor Fuel Development and Qualification Program, which supports the development and qualification of tristructural isotropic (TRISO) coated particle fuel for use in high-temperature gas-cooled reactors. The goals of these experiments are to provide irradiation performance data to support fuel process development, qualify fuel for normal operating conditions, support development of fuel performance models and codes, and provide irradiated fuel and materials for post-irradiation examination and safety testing. Originally planned and named as separate fuel experiments, but subsequently combined into a single test train. AGR-5/6/7 will test low-enriched uranium oxycarbide (UCO – a heterogeneous mixture of uranium oxide and uranium carbide) TRISO fuel. The AGR-5/6 portion of the experiment will provide data to support qualification of the selected reference fuel design, while the AGR-7 portion will serve as a margin test, irradiating the fuel beyond normal operating conditions. During irradiation, the temperature in each capsule is controlled by varying the helium / neon gas mixture flowing through the capsule until the desired thermocouple temperature is reached. Further adjustments can be made by changing the lobe power and the neutron filter. Three neutron filters are available to use as the experiment burns up the fissionable fuel. A thermal finite element model has been created for the five capsules comprising the AGR-5/6/7 experiment. Heat rates from a physics analysis are imported into the model along with fast neutron fluence. Graphite shrinkage due to the fast neutron fluence is incorporated into the model. Gas gaps change as a function of fast neutron fluence. Radiation heat transfer is a major contributor in this model. This is a large model with more than 1 million finite element brick elements. More than 150 different parts are modeled in the finite element model and communicate with each other from a heat transfer sense. More than 50 thermocouples are used in the experiment and are compared to actual measurements. The experiment is composed of five separate stainless steel capsules all welded together. This paper presents a method used to predict the gas mixture in the event that all of the thermocouples fail in a particular capsule. Curve fitting of heat rates from previous cycles and projecting them into the future is the basis of the method.

36 MATERIALS SCIENCE↗

Real Time Flame Monitoring of Gasifier and Injectors

This project is a multistage effort with the final goal to develop a practical and reliable nonintrusive gasifier injector monitor to assess burner wear and need for replacement. The project team included the National Energy Technology Laboratory (NETL), Gas Technology Institute (GTI), North Carolina State University, and ConocoPhillips. This report presents the results of the sensor development and testing initially at GTI combustion laboratory with natural gas flames, then at the Canada Energy Technology Center (CANMET), Canada in the atmospheric coal combustor as well as in the pilot scale pressurized entrained flow gasifier, and finally the sensor capabilities were demonstrated at the Pratt and Whitney Rocketdyne (PWR) Gasifier and the Wabash River Repowering plant located in West Terre Haute, IN. The initial tests demonstrated that GTI gasifier sensor technology was capable of detecting shape and rich/lean properties of natural gas air/oxygen enriched air flames. The following testing at the Vertical Combustor Research Facility (VCRF) was a logical transition step from the atmospheric natural gas flames to pressurized coal gasification environment. The results of testing with atmospheric coal flames showed that light emitted by excited OH* and CH* radicals in coal/air flames can be detected and quantified. The maximum emission intensities of OH*, CH*, and black body (char combustion) occur at different axial positions along the flame length. Therefore, the excitation rates of CH* and OH* are distinct at different stages of coal combustion and can be utilized to identify and characterize processes which occur during coal combustion such as devolatilization, char heating and burning. To accomplish the goals set for Tasks 4 and 5, GTI utilized the CANMET Pressurized Entrained Flow Gasifier (PEFG). The testing parameters of the PEFG were selected to simulate optimum gasifier operation as well as gasifier conditions normally resulting from improper operation or failed gasifier injectors. The sensor developed under previous tasks was used to assess the spectroscopic characteristics of the gasifier flame. The obtained spectral data were successfully translated into flame temperature measurements. It was also demonstrated that the reduced spectral data could be very well correlated with very important gasification process parameters such as the air/fuel and water/fuel ratio. Any of these parameters (temperature, air/fuel, and water/fuel) is sufficient to assess burner wear; however, the tested sensor was capable of monitoring all three of them plus the flame shape as functions of burner wear. This will likely be a very powerful tool which should enable significant improvements in gasifier efficiency, reliability, and availability. The sensor technology was presented to the project's industrial partner (ConocoPhillips). The partner expressed its strong interest in continuing to participate in the field validation phase of GTI's Flame Monitor Project. Finally the sensor was tested in the PWR (Pratt & Whitney Rocketdyne) gasification plant located at GTI's research campus and at the ConocoPhillips industrial scale gasifier at Wabash River Indiana. The field trials of the GTI Gasifier sensor modified to withstand high temperature and pressure corrosive atmosphere of the industrial entrain flow gasifier. The project team successfully demonstrated the Gasifier Sensor system ability to monitor gasifier interior temperature maintaining unobstructed optical access for in excess of six week without any maintenance. The sensor examination upon completion of the trial revealed that the system did not sustain any damage and required minor cleanup of the optics.

01 COAL, LIGNITE, AND PEAT↗

High-speed phase contrast imaging of spray breakup of jet fuels under combusting conditions

X-ray phase contrast imaging is conducted at 90,517 Hz on a fuel spray to characterize the breakup of the bulk fuel into ligaments and individual droplets in a single-sector, swirl-stabilized combustor under reacting conditions. Phase contrast imaging is used to qualitatively assess spray breakup for two fuels: Jet-A, which represents a normal viscosity fuel, and a blend of JP-5 (64%) and farnesane (36% by volume), which represents a high-viscosity fuel, at three fuel-flow rates and two air inlet temperatures. Time-series images of the fuels show that atomization occurs much more rapidly at higher fuel pressure with thinner ligaments being rapidly shredded. The high-viscosity fuel is qualitatively observed to have markedly longer, thicker ligaments and larger droplet diameters after the primary breakup than the normal viscosity fuel. Using an image processing and droplet quantification strategy, the mean droplet velocity magnitudes were found to decrease with decreasing fuel pressure and fuel-flow rate. The increase in preheat temperature from 323 to 370 K results in an increase in the mean droplet velocity magnitude and a decrease in numerical average and Sauter mean diameter, indicating improved atomization. The high-viscosity fuel was found to have larger average droplet diameters at each condition than the normal viscosity fuel. The increased preheat is found to enhance the combustion efficiency, which is hypothesized to couple with the improved atomization due to the higher combustion temperatures. This indicates the importance of examining spray atomization and breakup under realistic combusting conditions for relevant fuels as the heat release directly couples with the atomization process.

42 ENGINEERING↗

Refining a Novel Process Monitoring Method to Safeguard Continuously Cycling Designs Using Isotopic Ratios

In advanced reactor (AR) designs, a common feature is continuous chemical processing and circulation of the nuclear material. This work bridges a significant measurement gap in safeguarding reactors with circulating fuel or continuous refueling by leveraging and building on the isotope ratio method first developed by our team under an FY21 Advanced Reactors International Safeguards Engagement (ARISE) project (Uribe et al. 2021). In circulating fuel designs, the radioisotope inventory changes from traditional effects (e.g., radioactive decay, fission) but also includes material transport due to pressure and temperature gradients. Such designs may also require regular or continuous additions or removals during operation, which significantly increases the rate of inventory change compared to traditional pressurized water reactor (PWR)s. Thus, directly tracking the nuclear inventory is ineffective since the isotopes are continuously added and removed. The isotope ratio method instead focuses on detecting changes to the input and output flows of radioisotopes. Previous work showed that for well-chosen pairs of isotopes, the isotopic ratio provides a sensitive and lasting indicator of deviation from normal conditions (e.g., startup, shutdown, diversion). The isotope ratio method is a process monitoring method with potential for application in for forward-looking approaches to International Atomic Energy Agency (IAEA) safeguards. The original process monitoring method was developed for a specific case—the decay tank of a thorium-fueled molten salt breeder reactor. In this expanded work, we explored other types of reactors and processes with nonstationary (e.g., flowing) nuclear material, which are difficult to safeguard with traditional methods because of the transient nature of the systems. The goal of the present work is to generalize the isotope ratio method for use in processes with continuously flowing nuclear material. All continuous processes have an average time for isotopes to be replaced in the system. The isotope ratio method works by choosing radioisotopes with half-lives both above and below the processing time. The present work seeks to explore which isotopes are suitable for the method by simulating the nuclear inventory, radioisotope emissions, and detector responses for several classes of advanced reactors. While the method can in principle be applied to other processes (e.g., enrichment or reprocessing facilities), the present work limits scope to ARs with continuously flowing fuel. Section 2 details the mathematics supporting the isotope ratio method, and Section 3 introduces the representative ARs selected for this work. Section 4 discusses how each reactor was analyzed, and Section 5 showcases the results for each representative reactor. Finally, Section 6 provides concluding remarks and suggests pathways for further analysis.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Synthesis of zinc ultrafine powders via the Guen–Miller flow-levitation method

Zinc ultrafine powders (UFPs) with the average particle size of 0.175 to 1.24 μm are synthesized via the flow-levitation method. The peculiarities of the formation of zinc UFPs are considered with respect to the carrier gas properties (heat capacity, thermal conductivity, and diffusion coefficient), as well as the gas flow parameters (pressure and flow rate). The obtained zinc particles are studied via scanning electron microscopy and X-ray diffraction. The factors determining the crystal structure of zinc particles and their size distribution are discussed as well. The data on oxidation of zinc stored in unsealed containers under normal conditions are also presented.

36 MATERIALS SCIENCE↗

Redox Reactions of Reduced Flavin Mononucleotide (FMN), Riboflavin (RBF), and Anthraquinone-2,6-disulfonate (AQDS) with Ferrihydrite and Lepidocrocite

Flavins are secreted by the dissimilatory iron-reducing bacterium Shewanella and can function as endogenous electron transfer mediators (ETM). In order to assess the potential importance of flavins in Fe(III) bioreduction, we investigated the redox reaction kinetics of reduced flavins (FMNH2 and RBFH2) with ferrihydrite and lepidocrocite. The organic reductants rapidly reduced and dissolved ferrihydrite and lepidocrocite in the pH range 4-8. The rate constant k for 2-line ferrihydrite reductive dissolution by FMNH2 was 87.5 ± 3.5 M-1∙s-1 at pH 7.0 in batch reactors, and the k was similar for RBFH2. For lepidocrocite, the k was 500 ± 61 M-1∙s-1 for FMNH2, and 236 ± 22 M-1∙s-1 for RBFH2. The surface area normalized initial reaction rates (ra) were between 0.08 and 77 μmoles∙m-2∙s-1 for various conditions in stopped-flow experiments. Initial rates (ro) were first-order with respect to Fe(III) oxide concentration, and ra increased with decreasing pH. Poorly crystalline 2-line ferrihydrite yielded the highest ra, followed by more crystalline 6-line ferrihydrite, and crystalline lepidocrocite. Compared to a previous whole-cell study with Shewanella oneidensis strain MR-1, our findings suggest that ETM reduction by the Mtr pathway coupled to lactate oxidation are rate limiting, rather than heterogeneous electron transfer to the Fe(III) oxide.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗