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At least 973 records · Page 54

Dioctyl ether radiolysis under used nuclear fuel reprocessing conditions: Foundational knowledge for the development of sacrificial ligand grafts

Radiation-induced ligand destruction and concomitant degradation product formation is unavoidable under envisioned used nuclear fuel reprocessing conditions, and ultimately limits the recyclability of a given solvent system formulation. With this in mind, a novel approach to ligand innovation for advanced separations processes is in the design of tailored “protomolecules,” which when exposed to ionizing radiation undergo desired chemical transformations, thereby allowing for a reprocessing solvent system to advantageously evolve with absorbed radiation dose. Here we provide foundational knowledge for the time-resolved (electron pulse) and steady-state (cobalt-60 gamma) radiolytic behavior of dioctyl ether, a protomolecule grafting surrogate. Gamma irradiation of single-phase solutions of dioctyl ether (5–100 vol.%) in n-dodecane resulted in the loss of dioctyl ether (G = -0.72 µmol J –1 ) and the formation of octane (G = 0.11 µmol J –1 ) and octanol (G = 0.15 µmol J –1 ) degradation products, the latter of which is a known reprocessing phase modifier and radioprotectant. Further, these radiation-induced changes were attributed to direct radiation effects, for more concentrated dioctyl ether solutions, and indirect radiation effects, predominantly driven by the reaction of dioctyl ether with the dodecane radical cation, for which we report a second-order rate coefficient of k = (1.53 ± 0.05) × 10 10 L mol –1 s –1 . Under typical biphasic extraction (4.0 mol L –1 HNO 3 ) and strip (0.1 mol L –1 HNO 3 ) reprocessing conditions, gamma irradiation of 5 vol.% dioctyl ether solvent systems afforded negligible change in the rate of parent molecule destruction but promoted significant differences in the radiolytic behavior of its degradation products. These differences are attributed to their respective interactions with [dioctyl ether/HNO 3 /H 2 O] and [octanol/HNO 3 /H 2 O] adducts extracted into the organic phase. Overall, these results support the grafting of ether linkages to advanced separations ligands (e.g., modified diglycolamides).

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Monolithic ATF MiniFuel Sample Capsules Ready for HFIR Insertion

Several advanced nuclear fuel concepts are being considered throughout the nuclear industry. Implementation of these concepts could increase accident tolerance or enhance performance beyond the capabilities of the UO₂-based nuclear fuel currently in use. Qualification and deployment of any new fuel requires rigorous irradiation testing to demonstrate performance under representative normal and off-normal operating conditions. The traditional approach for qualifying new fuels requires exhaustive execution of many integral fuel tests. However, due to the long timeframe for executing these integral tests and the limited number of available materials test reactors, this approach is becoming impractical. To accelerate fuel qualification, Oak Ridge National Laboratory developed the MiniFuel irradiation vehicle for use in conducting accelerated separate effects irradiation testing of a wide range of nuclear fuel materials in the High Flux Isotope Reactor (HFIR). The first MiniFuel irradiations performed in the facility tested sol gel–derived uranium nitride kernels and tristructural isotropic (TRISO)-coated particle fuels. This report describes the preparation and assembly of the first set of monolithic MiniFuel irradiations conducted to support accident-tolerant fuel (ATF) development and accelerated fuel qualification. Two irradiation targets containing a variety of UO₂ and U₃Si₂ disk fuel specimens were fabricated and assembled for irradiation to burnups of 8-10 and 28-40 MWd/kg U. The target irradiation temperature is 450-550°C. Irradiation of U₃Si₂ will provide new data regarding the irradiation performance of a candidate ATF to complement current ATF-1 integral experiments being performed in the Advanced Test Reactor. UO₂ samples were included as a reference so that the results from the MiniFuel experiments can be compared with the extensive UO₂ fuel performance database. The monolithic MiniFuel capsules were successfully assembled, welded, and tested per HFIR requirements and are ready for insertion into the reactor. Pictures of the assembly process are included in this report. The experiment is planned for insertion into the HFIR during cycle 487 in April 2020.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Regenerative Fuel Cell System (Cooperative Research and Development Final Report, CRADA Number CRD-16-635)

Grid energy storage is required to maintain reliable electricity delivery from energy producers to their customers. As electrical loads on the grid change throughout the day, stored energy supplies electricity during increased power demand periods. Further, as more renewable and alternative energy sources are added, energy storage will maximize the usefulness of these technologies. Currently, the United States has over 24.6 GW of grid storage, about 2% of the total electrical production capacity. About 95% of energy storage comes from pumped hydro. However, pumped hydro energy storage is dependent on existing geographic features, making it difficult to integrate with widespread renewable energy sources. As energy demands continue to expand, and more renewable energy (i.e. wind and solar) is added to the grid, new energy storage technologies will be needed that are not dependent on geographic features. Battery technologies can provide energy storage for some applications, but are not economically well-suited for long duration charge/discharges, such as load-leveling of renewable energy. Consequently, development of new energy storage devices will augment the existing grid and reduce the capital investment in construction upgrades. As ever-increasing mandates for renewable energy are implemented, lower-cost energy storage solutions for renewable energy will be necessary to keep electricity costs low for consumers.

13 HYDRO ENERGY↗

A Vacuum Drying Study of Simulated Failed Nuclear Fuel (FY23)

This report documents work performed under the Office of Spent Fuel and Waste Disposition’s (SFWD’s) Spent Fuel and Waste Science and Technology program for the US Department of Energy (DOE) Office of Nuclear Energy (NE). This work was performed to fulfill Level 4 milestone M4SF-23OR010203013. Over the 70 years of light-water reactor (LWR) operation, fuel rod failures have occurred during reactor operation. Based on the Unified Database that SFWD maintains, there are ~5,400 LWR fuel rods that developed leaks during reactor operation of the >19 million rods operated. The Unified Database indicates that ~4,200 of these rods remain in the spent fuel pool, and ~1,200 are in dry storage canisters. It is expected that all failed rods are “waterlogged” in the spent fuel pool, meaning the inside of the rods contain some volume of water. There are two related objectives of this work. The first is to develop a simple and inexpensive experiment to better understand removal of water from inside failed spent nuclear fuel (SNF) rods, and the second is to develop a model to predict drying of simulated failed fuel in the simple experiment. Once a model captures the phenomenon in the simple experiment, it can be extended to predict drying under more prototypical conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Experimentally validated multiphysics modeling of fracture induced by thermal shocks in sintered UO 2 pellets

Uranium Dioxide (UO 2 ) fuel powers almost all commercial Nuclear Power Plants (NPPs) worldwide, generating carbon-free energy and contributing to the fight against climate change. UO 2 fuel incurs damage and fractures due to large thermal gradients that develop across the fuel pellet during normal and transient operating conditions. A comprehensive understanding of the underlying mechanisms by which these processes take place is still lacking. A combined experimental and computational approach is utilized here to quantify the behavior of UO 2 fuel fracture induced by thermal shock. Here, this work introduces both (1) an experimental study to understand the fuel fracturing behavior of sintered UO 2 pellets when exposed to thermal shock, and (2) a Multiphysics phase-field fracture model capable of simulating this process. Parametric studies were conducted to evaluate the effects of uncertainties in fracture properties on the fracture behavior of UO 2 due to thermal shocking. A set of energy release rate (or equivalently fracture toughness) and contract area (the part of the fuel pellet in direct contact with the cold bath) were able to capture the overall fracture trends of the corresponding experimental data. Our combined approach presents a new method for accounting for the effects of microstructure and sample size on the energy release rate/fracture toughness. The experimental data were collected from multiple experiments that exposed UO 2 pellets to high-temperature conditions (589–676 °C) followed by a quench in sub-zero water. This work demonstrates that joint experimental and computational efforts are able to advance the understanding of thermal fracture in the primary fuel source for existing and future NPPs.

36 MATERIALS SCIENCE↗

University of Missouri Research Reactor LEU Fuel Element Flow Test Conceptual Design

As part of the U.S. National Nuclear Security Administration’s (NNSA’s) mission to eliminate or minimize the civilian use of weapon-grade highly enriched uranium (HEU) fuels, the NNSA Office of Material Management and Minimization (M 3 ) Conversion Program is collaborating with six U.S. High Performance Research Reactors (USHPRR), including one critical facility, to convert from the use of HEU to low-enriched uranium (LEU) fuel. The M 3 conversion objectives for the USHPRR are to develop LEU fuel-element designs that will ensure safe reactor operations, as well as maintain the existing experimental performance of each facility. The work is being conducted through many interrelated activities that are being completed by stakeholders across organizations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Revised Point of Departure Design Options for Nuclear Thermal Propulsion

In an effort to further refine potential point of departure nuclear thermal rocket engine designs, four proposed engine designs representing two thrust classes and utilizing two different fuel matrix types are designed and analyzed from both a neutronics and thermodynamic cycle perspective. Two of these nuclear rocket engine designs employ a tungsten and uranium dioxide cermet (ceramic-metal) fuel with a prismatic geometry based on the ANL-200 and the GE-710, while the other two designs utilize uranium-zirconium-carbide in a graphite composite fuel and a prismatic fuel element geometry developed during the Rover/NERVA Programs. Two engines are analyzed for each fuel type, a small criticality limited design and a 111 kN (25 klbf) thrust class engine design, which has been the focus of numerous manned mission studies, including NASA's Design Reference Architecture 5.0. slightly higher T/W ratios, but they required substantially more 235U.

Nuclear Thermal Rockets↗

Comparative post-irradiation examination of high burnup U-19Pu-10Zr: Assessing steady-state irradiation behavior against historical and modeled fuel performance

Here, the development of next-generation sodium-cooled fast reactors necessitates comprehensive research on metallic fuels to maximize economic performance while ensuring safe operation. In this study, we investigated the steady-state irradiation behavior of two high burnup U-19Pu-10Zr fuel pins, DP-36 and DP-40, in preparation for planned safety testing. Post-irradiation examination (PIE) was performed to quantify fuel column elongation, regions of low-density at the top of the fuel column, pin deformation, fission product distribution, fractional fission gas release, microstructural evolution, and fuel constituent redistribution. Benchmarking against existing PIE data from U-19Pu-10Zr fuel pins irradiated in EBR-II revealed consistent patterns in fuel column elongation and cladding diametral strain. However, both pins exhibited longer low-density structures, and destructive examination of DP-36 revealed more complex constituent redistribution patterns compared to previously reported data for ternary fuel pins. The steady-state irradiation of both pins was also modeled using BISON. Comparisons of PIE results with modeled predictions showed overall agreement in fractional fission gas release but consistent overestimation of axial and radial swelling due to gaseous and solid swelling models. These findings underscore the critical importance of pre-test characterization on test and sibling pins to accurately capture steady-state fuel behavior ahead of transient testing, thus establishing a baseline for post-test comparison. Additionally, these analyses identified key data gaps that warrant further investigation to improve the understanding and prediction of fuel swelling, thereby enhancing the synergy between modeling and experimental efforts in supporting accident testing.

BISON↗

Low NO sub x heavy fuel combustor concept program phase 1A gas tests

The emissions performance of a rich lean combustor (developed for liquid fuels) for combustion of simulated coal gases ranging in heating value from 167 to 244 Btu/scf were assessed. The 244 Btu/scf gas is typical of the product gas from an oxygen blown gasifier, while the 167 Btu/scf gas is similar to that from an air blown gasifier. Although meeting NOx goals for the 167 Btu/scf gas, NOx performance of the rich lean combustor did not meet program goals with the 244 Btu/scf gas because of high thermal NOx, similar to levels expected from conventional lean burning combustors. The NOx emissions are attributed to inadequate fuel air mixing in the rich stage resulting from the design of the large central fuel nozzle delivering 71% of the total gas flow. NOx generation from NH3 was significant at ammonia concentrations significantly less tha 0.5%. These levels occur depending on fuel gas cleanup system design, However, NOx yield from ammonia injected into the fuel gas decreased rapidly with increasing ammonia level, and is projected to be less than 10% at NH3 levels of 0.5% or higher.

Cutrone, M. B.↗

BISON Development and Validation for Priority LWR-ATF concepts

Over the years, the Nuclear Energy Advanced Modeling and Simulation (NEAMS) (2015-2018, 2020) and Consortium for Advanced Simulation of Light Water Reactors (CASL) (2019) programs have provided support for development of Accident Tolerant Fuel (ATF) material models in the BISON fuel performance code. Since the beginning, the goal has been to utilize a multiscale modeling approach to gain a physical understanding of the fuel concepts of interest and to develop mechanistic models in the absence of a large amount of experimental data. This work builds upon that of previous years. In particular we present newly updated fission gas release models for both gas behavior in Cr 2 O 3 -doped UO 2 and U 3 Si 2 fuels, and a new creep model for U 3 Si 2 . The validation exercises completed last year are revisited with the latest models and the results updated. A brief summary of recent modeling activities for FeCrAl cladding is also provided.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Use of a Lignin-Based Admixture for Tailoring the Rheological Properties of Mortars for 3D Printing: Preprint

Efforts toward decarbonizing construction materials and industrial processes related to cement and concrete can be aided via multifaceted approaches that target alternative admixtures as well as precision control of fabrication. Chemical admixtures for water reduction have played a crucial role in the development of advanced concrete mixtures. Newer biomass processing techniques developed for aviation fuel production from corn stover biomass produce a more reactive lignin byproduct that is suitable for chemical modifications to mimic the properties of polycarboxylate ether admixtures with a smaller carbon footprint. The present study examines the use of lignin-based water-reducing admixture in cement pastes and mortar mixtures for 3D printing. The experimental program explores the use of different dosages of lignin-based admixture to produce 3D-printed samples with appropriate extrudability and buildability. The rheological characterization was performed to determine the flow curve of various mixtures. Finally, the heat of hydration of cement pastes was monitored via isothermal calorimetry to assess the impact of lignin-based admixtures on the hydration process of cement. The results of this study indicate that the use of biomass by-products, such as lignin-based admixtures have great potential to effectively control the fresh-state properties of cement-based materials.

bio-based admixtures↗

Accident-Tolerant Fuel

Advanced light water reactor (LWR) fuels have been developed incrementally for more than 60 years before the term Accident Tolerant Fuel (ATF) was created. There are many different categories of ATF concepts, which range from near-term marginal enhancements to fission gas release in fuel or hydrogen pickup in the cladding, to transformational fuel types with new engineered fission product barriers. In this work we characterize these different types of ATF, and give several important examples for each.We conclude that transformational ATF concepts have the greatest potential to enhance the traditional definition of defense-in-depth by enhancing current barriers and/or by providing additional barriers to fission product release. This objective can primarily be achieved by introducing a new fission product barrier that enhances defense-in-depth by design, for example the added barriers to fission product release in some engineered ATF concepts. We recommend future gap analyses and a phenomena identification and ranking to assess the applicability of existing safe acceptable fuel design limits and the standard review plan to specific ATF concepts.

Brown, Nicholas↗

Experimental Evaluation of the Fast-Neutron Passive Collar (FNPC) Performance (Interim Report)

This report represents a deliverable in the Safeguards Technology WBS # Project Title, 24.1.3.1, Task 3 (Report on laboratory-based performance testing of the FNPC). A new, simplified method for the verification of the 235 U mass in fresh LEU fuel assemblies that is relatively independent of burnable poison content is being developed. LWR fresh fuel is currently verified using the uranium neutron coincidence collar (UNCL), which relies on an AmLi source to induce fission in the 235 U. AmLi neutrons are slowed down in polyethylene, so the induced fission is primarily due to thermal neutrons. Burnable poisons, which are added to nuclear fuel assemblies to extend the lifetime of the fuel, absorb neutrons that would otherwise have induced fission in the fuel, thereby reducing the neutron count rate and thus the measured 235 U mass. To remove this bias factor a correction is applied based on the operator’s declared burnable poison content. The new technique uses 238 U spontaneous fission in LWR fresh fuel rods to self-interrogate the 235 U mass. The 238 U spontaneous fission neutrons have a hard neutron energy spectrum, which means that the technique is less sensitive to burnable poisons than the AmLi based systems. This project has continued the work done over the past two years to study this new technique using the optimized 3 He based fastneutron passive collar (FNPC). Fabrication of the FNPC has been completed and measurements are in progress using the LANL mockup PWR fuel assembly. Also, preliminary evaluations of advanced analysis techniques and unattended mode operation have been performed. In FY18, the 3 He tube based detector was compared with a 10 B sealed cell based detector for the same set of PWR fuel assemblies in the Rodeo-II program. The results were that the optimized 3 He detector had higher efficiency and less weight than the 10 B based system where both systems had about the same cost. Thus, the FY19 work continued exclusively with the 3 He based detector; although, either system had the potential for future applications. However, the high efficiency of the FPNC (~24%) is critical for precise measurements of the triples rate necessary in the multiplicity advanced analysis technique which can solve for the burnable poison content.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

ACE001: Heavy-Duty Diesel Combustion (Sandia National Laboratories)

Regulatory drivers and market demands for lower pollutant emissions, lower carbon dioxide emissions, and lower fuel consumption motivate the development of cleaner and more fuel-efficient engine operating strategies. Most current production engines use a combination of both in-cylinder and exhaust emissions control strategies to achieve these goals. The emissions and efficiency performance of in-cylinder strategies depend strongly on flow and mixing processes associated with fuel injection and heat losses.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

An Evaluation of a Neutron Time Correlated Interrogation Method for Measurement of Fissile Content in Research Reactor Spent Fuel Assemblies

There are many research reactors worldwide that have been, or are being converted from the use of high enrichment uranium (HEU) to low enrichment uranium (LEU, < 20% enriched). The verification of fissile content and initial enrichment of the spent fuel is needed for the effective safeguards of the fuel. The advanced experimental fuel counter (AEFC) was developed for the measurement of spent fuel rods and assemblies from research reactors for safeguards verification. This measurement system contains components for active neutron interrogation, passive neutron totals counting, neutron coincidence counting, and gross gamma-ray counting. This report presents the first application of the time correlated interrogation technique for the measurement of the 235 U content in research reactor spent fuel assemblies. The technique, called time correlated induced fission (TCIF), uses a 252 Cf neutron source to irradiate the fuel assembly, and the subsequent induced fission events in the fissile material are measured by coincidence counting. The doubles rates are enhanced by having the neutron trigger events from both the 252 Cf source and the induced fission neutrons in the same time gate in the coincidence analysis. The average neutrons per fission of the 252 Cf source is 3.76 and the induced fission neutrons for 235 U is 2.44, so the number of neutrons that are produced is higher than for random neutron interrogation. This high effective neutron number increases the multiplicity counting rates and reduces the statistical error. The background coincidence counts from the 252 Cf are reduced by the water in the sample cavity and the polyethylene surrounding the 3 He detector tubes. This method of active neutron interrogation has been applied to the measurement of spent research reactor (IRT) fuel assemblies. The advanced experimental fuel counter (AEFC) was used to compare the TCIF method with the typically used AmLi neutron interrogation source that emits neutrons that are random in time. The statistical uncertainty for the use of the random neutron source (AmLi) and the time correlated source ( 252 Cf) for spent fuel interrogations was evaluated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗