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DOE OSTI2021

HFIR SiC Bowing Test Ready to Insert

This report describes the successful assembly of a High Flux Isotope Reactor (HFIR) irradiation experiment designed to assess radiation-induced lateral bowing of silicon carbide fiber–reinforced, silicon carbide matrix composite (SiC/SiC) components under a radial fast neutron flux gradient. Excessive bowing of a SiC/SiC channel box in a boiling water reactor could potentially interfere with control blade movements. Similar concerns exist for SiC/SiC fuel cladding in light water reactors. The experiment described herein will provide experimental validation of the structural response of a miniature SiC/SiC channel box and tube specimens with pressurized water reactor diameters during irradiation. The significant radial fast neutron flux gradients that exist in the permanent reflector of HFIR were characterized using detailed three-dimensional neutronic calculations. The three-dimensional displacement damage dose rate profile and the resulting volumetric swelling in SiC were used as inputs to structural analyses that predicted the deformation and stresses in the channel box specimen. The specimens were thoroughly characterized prior to irradiation using traditional dimensional inspection and surface profilometry so that these measurements can later be compared with similar measurements that will be made post-irradiation to determine radiation-induced deformations. Furthermore, fine engraving markers were inscribed along all outer surfaces of the specimen and mapped using a digital microscope and a three-dimensional stage. This technique allowed for accurate measurements of the marker spacings, which can be compared with similar measurements that will be made post-irradiation to provide local radiation-induced strain mapping. The experiment was successfully assembled and is scheduled for insertion during HFIR cycle 492, which is currently scheduled to run from May 25, 2021 to June 18, 2021.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

Experiments to Measure the Inversion Point of the Isothermal Reactivity Coefficient in a Water-Moderated Pin-Fueled Critical Assembly at Sandia [Slides]

Two experiment series are planned to measure temperature effects in the Sandia Critical Experiments. The first series (IER-304) will measure the critical size of a fuel rod configuration at several temperatures. The second series (IER-452) will measure the inversion temperature of the isothermal reactivity coefficient in the Sandia critical assembly. Each experiment in the second series will be preceded by one or more experiments in the first series. This presentation addresses the conceptual design of the inversion temperature experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Verification of Spent Fuel Inside Dry Storage Casks by Cask Top Fast Neutron Mapping (FY2023 Mid-Year Report)

This project is developing a prototype scanner array verification system for detection of missing fuel assemblies in spent-fuel storage casks. The prototype consists of six fast-neutron scintillator detectors mounted to a linear actuator frame that is placed on the top of a spent fuel cask to scan across all fuel assembly positions. The scanner array was assembled and tested at LLNL in FY2022. A field test schedule has been requested at the Idaho National Laboratory (INL) Cask Farm site for FY2023. Note that the Cask Farm contractor determines this scheduling and not INL directly. Further system automation will be designed and implemented with the goal of obtaining a level of system operation that meets IAEA needs. This includes integration of the scanner array and data-acquisition control software into a single interface for operator use. In addition, commercial operators and the IAEA may have special requirements for portability, shipping, lifting, and installation. Prior to the Field Test at INL, the system will be operated at LLNL to exercise lifting procedure and linear actuators, monitor stability of detector energy and pulse-shape discrimination calibration, and test system software integration efforts. Following the Field Test, we will present results and discuss the technology with the IAEA. We will incorporate additional improvements to the system based on lessons learned from the field test and feedback from the IAEA. If successful, the technology can be transferred to the IAEA or other stakeholders for assessment.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

Pure-Water-Fed Forward-Bias Bipolar Membrane CO 2 Electrolyzer

Coupling renewable electricity to reduce carbon dioxide (CO 2 ) electrochemically into carbon feedstocks offers a promising pathway to produce chemical fuels sustainably. While there has been success in developing materials and theory for CO 2 reduction, the widespread deployment of CO 2 electrolyzers has been hindered by challenges in the reactor design and operational stability due to CO 2 crossover and (bi)carbonate salt precipitation. Herein, we design asymmetrical bipolar membranes assembled into a zero-gap CO 2 electrolyzer fed with pure water, solving both challenges. By investigating and optimizing the anion-exchangelayer thickness, cathode differential pressure, and cell temperature, the forward-bias bipolar membrane CO 2 electrolyzer achieves a CO faradic efficiency over 80% with a partial current density over 200 mA cm –2 at less than 3.0 V with negligible CO 2 crossover. In addition, this electrolyzer achieves 0.61 and 2.1 mV h –1 decay rates at 150 and 300 mA cm –2 for 200 and 100 h, respectively. Postmortem analysis indicates that the deterioration of catalyst/polymer– electrolyte interfaces resulted from catalyst structural change, and ionomer degradation at reductive potential shows the decay mechanism. Furthermore, all these results point to the future research direction and show a promising pathway to deploy CO 2 electrolyzers at scale for industrial applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

ROADRUNNER MiniFuel Experiment: Readiness for Insertion

The Research On ADvancing the peRformance of UraNium Nitrides in Extreme enviRonments (ROADRUNNER) campaign is a collaborative irradiation experiment designed to evaluate the performance of uranium nitride (UN) fuel fabricated with controlled variations in density and impurity content. Oak Ridge National Laboratory’s MiniFuel irradiation platform and the High Flux Isotope Reactor (HFIR) are being used to irradiate six targets containing 36 UN miniature disks. These targets have been assembled to systematically investigate burnup and temperature effects under accelerated irradiation conditions. This report documents the finalized test plan, describes the experiment assembly and subcapsule integration process, and confirms the readiness of all ROADRUNNER targets for HFIR insertion. All targets have passed quality control procedures, and five have begun irradiation. The campaign will provide critical performance data to support fuel model validation and future UN qualification efforts.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

ROADRUNNER MiniFuel Experiment: Readiness for Insertion

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Characterizing the seismic response of a molten salt nuclear reactor

Abstract One Generation IV nuclear reactor, which uses a fluoride salt as a coolant, graphite reflector blocks as a moderator, and circulating buoyant TRISO pebbles as fuel is at an advanced stage of development. To characterize the seismic behavior of components of this reactor, validate numerical models for analysis, and develop recommendations for design, a set of earthquake‐simulator experiments on a scaled model of the reactor vessel and its internals was executed on a six‐degree‐of‐freedom earthquake simulator. The model was seismically isolated at its base using two types of spherical sliding bearings. The scaled model involved representations of the prototype reactor vessel, core barrel, reflector blocks, coolant, and spherical fuel pebbles. The material and geometric properties of different test components were selected based on a dynamic similitude scaling analysis and an approximate length scale of 0.4. Four sets of three‐component earthquake motions were used as inputs for testing. Instrumentation on the test specimen recorded the dynamic responses of the outer vessel, core barrel, and reflector‐block assembly, the hydrodynamic responses (sloshing and hydrodynamic pressure) of the liquid coolant, pebble consolidation under earthquake shaking, and the behavior of the isolation systems. This paper describes the design of the experiments and presents key results from the tests. The dynamic responses of the outer vessel, core barrel, and the reflector blocks revealed that the components responded as a unit for the intense shaking used in the experiments. The sloshing response of the fluid in a thin annulus near the perimeter of the vessel was heavily damped. The change in the packing fraction of the pebble bed under repeated, intense 3D earthquake shaking was less than 3%. Seismically isolating the vessel substantially reduced demands on its internal components.

Engineering↗

DOE OSTI2023

A computational parametric study of ducted fuel injection implementation in a heavy-duty diesel engine

Experiments have shown that ducted fuel injection (DFI) effectively reduces soot emissions from direct-injection diesel engines. Although many computational studies have evaluated DFI’s spray development and soot reduction mechanisms in constant volume chambers, only limited computational work on internal combustion engines exists. The DFI duct assembly changes the engine’s in-cylinder flow, spray, and combustion development. Therefore, current production engine designs might not be optimal for achieving the best engine performance with DFI. Here, this work conducted an extensive numerical study to evaluate how parameter changes affect DFI performance. The parameters include swirl ratio, piston geometry, compression ratio (CR), number of injector orifices, split injection strategy, and exhaust gas recirculation (EGR) in a heavy-duty diesel engine utilizing DFI. The combustion and soot emission data from the Sandia compression ignition optical research engine were used for model validation. Simulations showed that an increased swirl ratio resulted in more intense jet flame-piston interaction, slowing down the combustion heat release during the late combustion stage and leading to lower indicated thermal efficiency (ITE) due to higher exhaust losses. A piston-bowl design with a reentrant inner piston edge yielded the highest thermal efficiency, due to the reduced cylinder head heat transfer loss. Additional injector orifices led to higher efficiency owing to a more advanced combustion phasing. Nevertheless, the maximum pressure rise rate (MPRR) and oxides of nitrogen (NO x ) emissions also increased with the number of injector orifices due to more rapid heat release and higher combustion temperature. Implementation of a split injection strategy combined with a higher EGR rate effectively inhibited the excessive MPRR and NO x formation. In general, the study concluded that DFI is not sensitive to most parameter changes but will benefit from future parameter optimization.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2021

Results of the 2018 Wood Stove Design Challenge

The 2018 Wood Stove Design Challenge was an international design competition which sought to identify top performing residential wood stoves based on automation. To prepare for the event, the Northeast States for Coordinated Air Use Management (NESCAUM) developed a testing protocol that challenged the stoves by testing them in more field-like conditions—capturing emissions from start-up, reloading a stove, and the use of larger piece sizes. Flue gas emissions were measured using a combination of in-stack and novel dilution sampling methods, as the event occurred on the National Mall in Washington D.C. in a non-laboratory setting. Particulate matter (PM), carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were measured from three stoves in real-time. A combustion efficiency was also calculated for each stove in real-time. Measured PM emission rates ranged between 1.8 and 8.0 g/hr for all stoves and operating conditions, with the highest emissions being measured during cold start in all cases. The test average PM emission rates were 2.4, 4.0, and 2.4 g/hr for stoves A, B, and C, respectively. Results showed emissions measured during transient operations, which are often excluded in current certification methods, can be significantly higher than steady-state periods—echoing other studies and highlighting the importance of testing in various operational modes for more realistic emission estimates. Additionally, the stoves had overall CO emission rates of 48.8, 284.8, and 100.8 g/hr, for stoves A, B and C, respectively. Calculated PM and CO emission factors overall were low considering the testing protocol sought to follow more challenging yet realistic practices in terms of fuel loading and operating procedures. The overall estimated combustion efficiency for stoves A, B, and C was 85%, 78%, 76%, respectively and in all cases was lowest during the cold start period.This report details the successfully proposed and assembled instrumentation that was relatively portable for field-site testing and the results of the emissions measurements for the 2018 Wood Stove Design Challenge competition. Overall, the repeatability of each stove was favorable with coefficients of variation (COV) ranging from 7 to 15% for measured PM concentrations.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2025

High Pressure Hydrogen Nozzle Assembly and Dispenser for Heavy Duty Vehicles (Final Technical Report)

Electricore, Inc. along with partners Bennett Pump Company (Bennett), WEH Technologies, Inc. (WEH), National Renewable Energy Laboratory (NREL), and Quong & Associates, Inc. (QAI) have developed a high-pressure hydrogen nozzle assembly and dispenser for heavy-duty (HD) vehicles. The system was installed, tested and demonstrated at NREL’s Hydrogen Infrastructure Testing and Research Facility (HITRF). The system was designed to have a maximum operating pressure of 87.5 MPa and an approximate average flow rate of 10 kg/min over 10 minutes at fuel temperatures of -40°C. To further develop the specifications and design of the system, the team performed an industry survey to ensure the system met the needs of potential users.

08 HYDROGEN↗

DOE OSTI2021

Modeling and Analysis for Spent Nuclear Fuel Seismic Testing

Note: This is the final public release version of PNNL-31671 Draft, which was previously released to the sponsor for review. The intent is the public release version will be PNNL-31671. There are no significant changes from the earlier draft version. This unlimited distribution report is the deliverable for M3SF-21PN010202014: Modeling and Analysis for Spent Nuclear Fuel Seismic Testing. This report summarizes the modeling, analysis, and test plan support completed by Pacific Northwest National Laboratory for the spent nuclear fuel dry storage system seismic test plan through May of 2021. Test plan preparation is planned to continue until the seismic test is completed in July of 2022. This report covers preliminary structural dynamic model development and computer-aided design of test hardware. Based on preliminary modeling, the strongest earthquakes under consideration in this test program provide mechanical loading on the spent nuclear fuel that is comparable to the 30 cm cask drop scenario, although the loads do not appear to be strong enough to cause significant permanent deformation of the fuel assembly spacer grids. The potential for grid deformation during the test will be assessed when the proposed shake table motion becomes available. The weakest earthquakes considered in this test are expected to be comparable to the mechanical loads witnessed in the multimodal transportation test of 2017. The horizontal canister system is predicted to provide nearly-uniform loading condition on the fuel assemblies it contains, while the vertical cask system is predicted to cause non-uniform dynamic loads on the fuel assemblies. In the horizontal case, gravity keeps the fuel assemblies in contact with one basket wall surface unless the loads are strong enough to cause a separation. In the vertical case, the fuel assemblies are relatively long and slender, and seismic motion in the anticipated test range is predicted to cause the assemblies to lean, tilt, and impact the basket walls throughout the seismic event. These gap closures are a nonlinear force transmission condition, so the vertical system is expected to have more variation and variability than the horizontal system. While the horizontal system is expected to have a relatively more linear response than the vertical system, there is still the potential for nonlinear behavior in the horizontal system because the fuel assemblies are free to slide, bounce, and impact the basket walls if the seismic loads are strong enough. One major conclusion of this study is that the use of mixed fuel assemblies in the canister will be acceptable. There are differences in overall system response when the mass, center of gravity, or gaps are changed, but the changes in response are within the bounds of a system that contains completely homogeneous fuel assemblies. One important observation is that the loading for each individual fuel assembly within the vertical canister is expected to be different from that of the others because of nonlinearities in the system. The horizontal canister system is expected to have a more uniform and more predictable response than the vertical canister, making variations in fuel assembly characteristics easier to account for. One important recommendation that comes from this modeling work is to repeat some of the strongest shake tests at different angles, particularly for the vertical cask system. Modeling predicts that strong seismic motion will cause the fuel assemblies to close initial gaps and impact the fuel basket walls when the canister is in the vertical cask configuration. Each shake test will impose a pre-defined three-dimensional time history on the cask system.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Submersible Multistage Centrifugal Pump for Versatile Test Reactor Cartridge Test Loop

Submersible multistage centrifugal pumps are ideal for pumping in narrow confined spaces and achieving necessary head pressures and flow rates. Once a diameter is determined then manipulation of the number of stages and motor speed are all that are required to meet desired flow conditions. The Versatile Test Reactor (VTR) closed loop cartridge systems will need forced convection cooling independent of the main reactor. A multistage centrifugal pump can meet the necessary flow rates and pumping pressures while minimizing space taken. The pump considered for this work was based off a deep well submersible pump, a variation of a multistage centrifugal pump. We experimented with two pump sizes, 5 cm (2 inch) and 7.5 cm (3 inch) diameters. These diameters were chosen to fit into the inner diameter of standard 5 and 7.5 (2 and 3 inch) Schedule 40 pipe, respectively. This made the design for the test loop both simpler and less expensive as the need for an engineered pump housing was eliminated. Initial test cartridge planning indicated space for only a 5 cm (2 inch) diameter pump, though early testing of this size showed the need for an abnormally high-speed and high-power motor. Fine tuning of the cartridge design allowed a pump size increase to 7.5 cm (3 inches), which was the pump size most extensively tested in this work. The test loop is composed of various sizes of PVC and aluminum piping components in a loop configuration. The pump is driven by a Pittman 250 W (1/3 horsepower) electric motor with maximum speed of 3,450 RPM. Testing consisted of running the pump at a constant motor speed while varying a control valve to restrict flow through the loop, with differential pressure and flow rate recorded. This was done for one and two stage configurations for the 5 cm (2 inch) diameter impeller design and one, two, and three stage configurations for the 7.5 cm (3 inch diameter) impeller design, respectively. Due to pumping power requirements, two and three stage 7.5 cm (3 inch) diameter impeller testing at higher flowrates lowered the motor speed substantially. In regions where motor speed could not be maintained constant, the data were discarded. The test loop was also reconfigured to allow for the pump to be tested for pressure drop in a stalled or inoperable (0 RPM) flow condition. Demonstration of adequate natural convection cooling of the test cartridge fuel type is necessary under accident conditions, and this will depend upon the flow resistance through the impeller assembly when the pump is not operating. Thus, accurate knowledge of the effective impeller assembly loss coefficient is important for safety evaluations. The test loop was modified to provide water inlet and outlets on either side of the pump impeller stack, and a metered flow of lab water was provided in order to measure the pressure drop across the cartridges as a function of flowrate. Data from the pump head curve testing developed as part of this work and supported by analysis using pump head affinity laws indicates that a three stage 7.5 cm (3 inch) pump impeller design will meet target requirements for coolant flow within the VTR cartridge sodium cartridge at full power conditions [1] with margin; this corresponds to a flowrate of 45 l/min (12 gpm) at a pressure drop of 6.1 m (20 feet) of water head. The results of the pressure loss measurements across the impeller assembly when the pump is stationary (i.e., at 0 RPM) indicate that the pressure loss coefficient is 0.921 for a two impeller stack configuration; this value is calculated based on the flow velocity through the minimum available flow area within a single stage of the impeller which corresponds to 1.4 cm2.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2023

Amino-tethering synthesis strategy toward highly accessible sub-3-nm L1 0 -PtM catalysts for high-power fuel cells

Because of the poor accessibility of embedded active sites, platinum (Pt)-based electrocatalysts suffer from insufficient Pt utilization and mass transport in membrane electrode assemblies (MEAs), limiting their performance in polymer electrolyte membrane fuel cells. Here, we report a simple and universal approach to depositing sub-3-nm L1 0 -PtM nanoparticles over external surfaces of carbon supports through pore-tailored amino (NH 2 )-modification, which enables not only excellent activity for the oxygen reduction reaction, but also enhanced Pt utilization and mass transport in MEAs. Using a low loading of 0.10 mg Pt ∙cm -2 , the MEA of PtCo/KB-NH 2 delivered an excellent mass activity of 0.691 A∙mgPt -1 , a record-high power density of 0.96 W∙cm -2 at 0.67 V, and only a 30-mV drop at 0.80 A∙cm -2 after 30,000 voltage cycles, which meets nearly all targets set by the Department of Energy. Finally, this work provides an efficient strategy for designing advanced Pt-based electrocatalysts and realizing high-power fuel cells.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

DOE OSTI2022

PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises

Proton-exchange membrane fuel cells (PEMFCs) are efficient and clean hydrogen energy technologies for transportation and stationary applications. Highly active and durable low-cost cathode catalysts for the oxygen-reduction reaction (ORR) under challenging acidic environments are desperately needed to address the cost and durability issues of PEMFCs. The most promising platinum group metal (PGM)-free catalysts for the ORR in acidic media are atomically dispersed and nitrogen-coordinated metal site catalysts denoted as M–N–C, M = Fe, Co, or Mn. Due to significant efforts in the past few decades, these catalysts have demonstrated much-improved ORR activity and promising initial fuel cell performance approaching traditional Pt/C catalysts. However, the insufficient long-term stability (up to 5000 h) under PEMFC operation represents a primary technical barrier to making current PGM-free catalysts less viable yet in PEMFCs. In this Account, we highlight recent advances in synthesizing efficient PGM-free catalysts for the ORR in PEMFCs, emphasizing effective strategies to improve mass and intrinsic activity and the possible degradation mechanisms. In particular, a chemical doping method based on the zeolitic imidazolate framework (ZIF)-8 represents the key to developing efficient M–N–C catalysts containing atomically dispersed and nitrogen-coordinated single metal active sites (i.e., MN 4 ). The newly acquired understanding of the formation mechanism of MN 4 active sites during the thermal activation and its correlation to catalytic properties guide the rational catalyst design rather than relying on current trial-and-error approaches. Considerable efforts have further been invested in increasing the active site density and enhancing intrinsic activity by regulating carbon-phase structures and the local coordination environment. Furthermore, these highly active catalysts usually suffer from significant activity loss during the ORR. Therefore, breaking the activity–stability trade-off is the key to simultaneously achieving activity and stability in one catalyst, which is discussed on the basis of our recent successes in regulating local carbon structures surrounding active single metal sites. Significant research efforts toward understanding the degradation mechanisms and improving the lifetime of PGM-free catalysts are still crucial for viable applications in the future. Novel electrode designing strategies are needed to translate the PGM-free catalysts’ ORR activity to solid-state electrolyte-based membrane electrode assemblies (MEAs) with robust three-phase (i.e., gas–liquid–solid) interfaces for efficient charge and mass transports for performance improvement. On the basis of our effort at the University at Buffalo supported by ElectroCat Consortium associated with U.S. DOE’s Hydrogen and Fuel Cell Technologies Office, we provide a perspective on PGM-free cathode catalysts concerning remaining bottlenecks and future opportunities, aiming to inspire the community in both mechanistic understanding and technological development.

08 HYDROGEN↗

DOE OSTI2022

Management of the Three Mile Island Unit 2 Accident Corium and Severely Damaged Fuel Debris (Rev. 2)

The Three Mile Island, Unit Two (TMI-2) pressurized water reactor core underwent a significant meltdown in 1979 due to an untimely combination of maintenance problems that led to a loss of feedwater, followed by a series of operational misunderstandings and errors. Primary coolant discharging through a malfunctioning valve represented what was analyzed as a “small-break” loss-of-coolant accident (LOCA) and ultimately became a full core meltdown. The melted core recovery process required the development of a wide array of tools. After approximately three years of water management and other cleanup actions, the first views of the core revealed a much higher degree of damage than previously expected. Approximately 62 metric tons of the core had melted, leaving only 42 of the 177 fuel assemblies standing with fuel rods intact. The core to be recovered was composed of loose, gravel-like and granular particulate material and a central solidified mass of formerly molten fuel. Molten fuel had also penetrated some of the pressure vessel internals and resolidified below the main core support structure. Robotic tools that had been designed for the task were of limited effectiveness due to the range of material types and phases.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Management of the Three Mile Island Unit 2 Accident Corium and Severely Damaged Fuel Debris (Rev. 2)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Integrated protonic ceramic electrochemical cell for sustainable energy economy using water-energy nexus framework

Reliance on fossil fuels will continue for the next decades even though there are global pushes away from it to mitigate the overarching climate challenge, most especially by its highest consumers and availability. While there is a hastening global shift away from fossil fuel, integrating its assets into this technology helps limit the risk and future losses of stranded assets and reduce the cost of investment in the new technologies. Moreover, the generation of electricity from intermittent renewable sources like solar and wind has witnessed a significant surge in recent years, leading to a pressing demand for practical energy storage systems. Electrical energy storage is anticipated to play a pivotal role in the future global energy system, facilitating load-leveling operations to support the greater integration of renewable and distributed generation. Reversible electrochemical cells (RECs) offer a promising option for addressing the fossil fuel assets integration and energy storage challenges through the interconversion between electrical and chemical energy and concurrent utilizing carbon emission. In their electrolysis mode, the RECs convert electricity into durable, storable, and portable valuable chemical fuels such as syngas and methane. Conversely, the produced chemical fuels can be used as reactants in the fuel cell mode to generate electricity on demand with minimal (hydrocarbons) or zero when H2 or NH3 is used emissions. However, a challenging goal for this type of technology remains to achieve optimal operation and high roundtrip efficiencies, which has hindered the deployment of previous electrochemical cells. This dissertation demonstrates how reversible protonic ceramic electrochemical cells (RePCECs) can be integrated with fossil fuel power plants and renewable energy sources as a potential energy storage system. In this work, integrated RePCEC systems are designed and examined using computational modeling at scales to determine appropriate system configurations and operating conditions that achieve high roundtrip efficiencies. Cell level design of the PCEC is the first approach, several cells are assembled for the stack level model that is integrated into combined cycle powerplant and solar photovoltaic for the system level model. After critical literature review, this answered the operational and integration research questions proposed to address these challenges. The designed systems perform two functions, utilizing captured CO2 and storing renewable energy through co-electrolysis of steam and CO2. The co-electrolysis reaction involves endothermic water electrolysis and exothermic methanation reaction. To enhance high roundtrip efficiency, there is a need for thermal balance and management in the electrolysis mode. This involves operating the RePCEC stack under conditions that favor methane production to balance out heat needed by water electrolysis, it crucial for the RePCEC system operation. Methanation is enhanced by low temperatures. Leveraging on fabricated BCZYYb-electrolyte RePCEC, the cell model designed revealed that the optimum temperature for methane production is 450℃ at atmospheric pressure. Thus, to achieve optimum system performance, operating in the temperature range 450-525℃ is recommended at the given configuration, combining between the optimum temperature for methane production and temperature for the optimum stack roundtrip efficiency. Configuration with carbon capture system and purge stream is the optimum configuration from the seven conceptualized and evaluated. The modeling outcomes include a thermodynamic examination of integrated RePCEC systems, calibration of cell and stack level models, and steady-state simulation and integration into a 600MW combined cycle power plant retrofitted with two two-stage membrane-based carbon capture system and a wastewater treatment and recovery unit. At 100% powerplant loading, the stack and system roundtrip efficiencies are 72% and 51.37% respectively. Adding a purge stream for produced hydrogen at the system downstream improves the efficiencies to 74 and 55.48% respectively. At atmospheric pressure and 525℃, the system model suggests that a stack roundtrip of 82% is achievable, and overall system efficiency increases by reducing the energy consumption by the balance of plant components for steam generation and storage. Economic analysis of the process gives levelized cost of methane as $2.24/MMBtu lower than the conventional production route that range between $3.46/MMBtu and $9.85/MMBtu. The lifecycle analysis shows that the global warming potential for the production of methane and hydrogen from the RePCEC system is 3.83 kg CO2 eq which is lower than 9.35 kg CO2 eq emission during steam methane reforming for hydrogen production. This answered both the environmental and economic concerns in the raised research question. The proposed RePCEC configuration and analysis carried out in this dissertation to address the surge in renewable energy and challenges with PCEC technology hold significant potential in achieving large-scale energy storage while simultaneously reducing carbon emissions. These advancements, coupled with suitable governmental policies and incentive programs, have the potential to economically disrupt the natural gas industries by using RePCEC systems for methane production, thereby making them more favorable for eventual implementation and commercialization.

25 ENERGY STORAGE↗

DOE OSTI2020

The Relationship Between Dose Rate and Decay Heat for Spent Nuclear Fuel Casks

Decay heat and dose rate are two important limits used for determining the allowable contents of spent fuel (SNF) in dry storage systems and transportation packages. While the decay heat limit is used to maintain fuel cladding integrity and ensure retrievability, dose rates are used to demonstrate compliance with regulatory requirements on radiation protection. Because both dose rate and decay heat result from decay of radioisotopes in SNF, this study is an attempt to examine the relationship between dose rate and decay heat for a given cask design. Dose rates were evaluated for 198 cask configurations, that include various SNF system designs (e.g., storage, transfer, transport), SNF characteristics (e.g., fuel types, burnup, cooling time), and loading maps (e.g., uniform loading, zone loading), while a constant decay heat was maintained. The decay heat was calculated using US Nuclear Regulatory Commission (NRC) Regulatory Guide (RG) 3.54, Revision 2, and verified using ORIGEN sequence within SCALE code system. The ORIGEN outputs were used as source terms in the dose analysis using 198 different configurations. A computer script was developed to calculate the cooling time necessary to achieve a given decay heat for a given enrichment, assembly average burnup, assembly mass, and in-core history using a rootfinder algorithm. Initially the computer script was developed to provide cooling time and burnup calculations directly to the analysis of dose rates and decay heats, so a comparison between Used Nuclear Fuel-Storage Transportation and Disposal Analysis Resource Data System (UNF-ST&DARDS) results and RG3.54 data was made; results are included in the appendix to this document. However, an iterative approach was used to compute cooling time, and its accuracy did not depend on the results of the RG3.54r2 algorithm, although the algorithm was still used. The results of the evaluation presented herein clearly demonstrate that a given decay heat does not correspond to a unique dose rate for a variety of cask and package designs. There is no clear pattern to develop a correlation between decay heat and the source terms. Depending on burnup, enrichment, cask type, and loading pattern, dose rates varied for the exact same decay heat—in some cases by 400% for a given cask. For cases in which decay heat was held constant through selection of the appropriate cooling time, dose rates would decrease with increasing burnup, and in other cases, dose rates would increase. The large variation in dose rates for a constant decay heat indicates that casks loaded based on decay heat—that is allowing any burnup, cooling time, and enrichment combinations that yield the qualified decay heat limit(s) —cannot ensure that an Independent Spent Fuel Storage Installation or a spent fuel transportation package will meet the regulatory limits set forth by the respective regulations, i.e., 10 CFR 72 or 10 CFR 71.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗