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DOE OSTI2013

Enhanced Accident Tolerant Fuels for LWRs - A Preliminary Systems Analysis

The severe accident at Fukushima Daiichi nuclear plants illustrates the need for continuous improvements through developing and implementing technologies that contribute to safe, reliable and cost-effective operation of the nuclear fleet. Development of enhanced accident tolerant fuel contributes to this effort. These fuels, in comparison with the standard zircaloy – UO2 system currently used by the LWR industry, should be designed such that they tolerate loss of active cooling in the core for a longer time period (depending on the LWR system and accident scenario) while maintaining or improving the fuel performance during normal operations, operational transients, and design-basis events. This report presents a preliminary systems analysis related to most of these concepts. The potential impacts of these innovative LWR fuels on the front-end of the fuel cycle, on the reactor operation and on the back-end of the fuel cycle are succinctly described without having the pretension of being exhaustive. Since the design of these various concepts is still a work in progress, this analysis can only be preliminary and could be updated as the designs converge on their respective final version.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Mobility assessment of the BCC and carbide phases in the C-Nb, C-U and Nb-U systems

Uranium carbides with refractory metal additions are considered for Gen IV nuclear reactors and nuclear thermal propulsion as fuels for their high-temperature and corrosion resistant properties. Understanding kinetic effects that dictate microstructural evolution during fabrication and operating conditions is essential to advance technological development of these fuels. This work presents the development of an atomic mobility database for C-Nb-U systems based off available experimental data supported with ab-initio methods. The mobility assessments and uncertainty quantification (using Markov chain Monte Carlo) were conducted in the Kawin software. Carbon diffusion is considered dominant, as metal diffusion is much slower, with niobium diffusion being even slower and rate limiting than uranium metal. We provide a comprehensive and self-consistent thermo-kinetic database that is validated by diffusion couple simulations through Kawin. In conclusion, this enables prediction of microstructural and phase evolution critical for the development and lifetime assessment of next generation nuclear fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Initiating a Roadmap for Solar Fuels R&D: Imagining Beyond Thermochemical Cycles

Sandia National Laboratories in collaboration with the National Renewable Energy Laboratory outline a framework for developing a solar fuels roadmap based on novel concepts for hybridizing gas-splitting thermochemical cycle s with high-temperature electro chemical steps. We call this concept SoHyTEC, a Solar Hybrid Thermochemical-Electrochemical Cycle. The strategy focuses on transforming purely thermochemical cycles that split water (H 2 O) and carbon dioxide (CO 2 ) to produce hydrogen (H 2 ) and carbon monoxide (CO) , respectively, the fundamental chemical building blocks for diverse fuels and chemicals , by substituting thermochemical reactions with high-temperature electrochemical steps. By invoking high-temperature electrochemistry, the energy required to complete the gas-splitting cycle is divided into a thermal component (process temperature) and an electrical component (applied voltage). These components, sourced from solar energy, are independently variable knobs to maximize overall process efficiency. Furthermore, a small applied voltage can reduce cycle process temperature by hundreds of degrees , opening the door to cost-effective solar concentrators and practical receiver/reactor de signs. Using the SoHyTEC concept as a backdrop, we outline a framework that advocates developing methods for automating information gathering, critically evaluating thermochemical cycles for adapting into SoHyTEC, establishing requirements based on thermodynamic analysis, and developing a model-based approach to benchmarking a SoHyTEC system against a baseline concentrating solar thermal integrated electrolysis plant. We feel these framework elements are a necessary precursor to creating a robust and adaptive technology development roadmap for producing solar fuels using SoHyTEC. In one example, we introduce high-temperature electrochemistry as a method to manipulate a fully stoichiometric two-step metal oxide cycle that circumvents costly separation processes and ultra-high cycle temperatures. We also identify and group water-splitting chemistries that are conceptually amenable to hybridization.

14 SOLAR ENERGY↗

DOE OSTI2016

Zurückgezogen: Glutarimidedioxime: A Complexing and Reducing Reagent for Plutonium Recovery from Spent Nuclear Fuel Reprocessing

Abstract Efficient separation processes for recovering uranium and plutonium from spent nuclear fuel are essential to the development of advanced nuclear fuel cycles. The performance characteristics of a new salt‐free complexing and reducing reagent, glutarimidedioxime (H 2 A), are reported for recovering plutonium in a PUREX process. With a phase ratio of organic to aqueous of up to 10:1, plutonium can be effectively stripped from 30 % tributyl phosphate (TBP) in kerosene into 1 m HNO 3 with H 2 A. The complexation‐reduction mechanism is illustrated with the combination of UV/Vis absorption spectra and the crystal structure of a Pu IV complex with the reagent. The fast stripping rate and the high efficiency for stripping Pu IV , through the complexation‐reduction mechanism, is suitable for use in centrifugal contactors with very short contact/resident times, thereby offering significant advantages over conventional processes.

Xian, Liang↗

DOE OSTI2016

Glutarimidedioxime: A Complexing and Reducing Reagent for Plutonium Recovery from Spent Nuclear Fuel Reprocessing

Xian, Liang↗

DOE OSTI2013

The Production Process, Thermophysical Properties, and Quality Assurance Process for the Provision of Enhanced Accident Tolerant Fuels: ORNL Rodlets for the ATR ATF-1 Experiment

The work documented in this report was performed under the Fuel Cycle Research and Development (FCRD) Program’s Advanced Fuels Campaign (AFC) FY13 Work Package Number FT-13OR020222, revision 0, “Route to production and qualification of FCM fuel - ORNL.” The sole milestone in this work package is M2FT-13OR0202221, “Report Documenting Production Process, Thermophysical Properties, and QA Process to be Applied to First Irradiation Batch of FCM Fuels,” due July 27, 2013. This report satisfies that milestone.

Bell, Gary L.↗

DOE OSTI2017

Heavy-Duty Low-Temperature and Diesel Combustion & Heavy-Duty Combustion Modeling

Regulatory drivers and market demands for lower pollutant emissions, lower carbon dioxide emissions, and lower fuel consumption motivate the development of clean and 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. Various diesel engine manufacturers have adopted close-coupled post-injection combustion strategies to both reduce pollutant emissions and to increase engine efficiency for heavy-duty applications, as well as for light- and medium-duty applications. Close-coupled post-injections are typically short injections that follow a larger main injection in the same cycle after a short dwell, such that the energy conversion efficiency of the post-injection is typical of diesel combustion. Of the various post-injection schedules that have been reported in the literature, effects on exhaust soot vary by roughly an order of magnitude in either direction of increasing or decreasing emissions relative to single injections (O’Connor et al., 2015). While several hypotheses have been offered in the literature to help explain these observations, no clear consensus has been established. For new engines to take full advantage of the benefits that post-injections can offer, the in-cylinder mechanisms that affect emissions and efficiency must be identified and described to provide guidance for engine design.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2021

Heavy-Duty Low-Temperature and Diesel Combustion & Heavy-Duty Combustion Modeling (FY 2018 Annual Progress Report)

Regulatory drivers and market demands for lower pollutant emissions, lower carbon dioxide emissions, and lower fuel consumption motivate the development of clean and fuel-efficient engine operating strategies. Most current production engines use a combination of both in-cylinder and exhaust emission 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. Both heavy- and light-duty engine/vehicle manufacturers use multiple-injection strategies to reduce noise, emissions, and fuel consumption. For both conventional and low-temperature diesel combustion, the state of knowledge and modeling tools for multiple injections are far less advanced than for single-injection strategies. Engine efficiency is limited to some degree by tradeoffs that must be accepted to meet particulate matter (including soot) emissions limits. Recent work on this project has filled some knowledge gaps on soot oxidation with multiple injections, and the current work for Fiscal Year (FY) 2018 addresses knowledge gaps on soot formation for multiple injections. While total in-cylinder soot is readily measured, discerning formation from oxidation is difficult. The FY 2018 experiments are designed to create in-cylinder conditions at the threshold of soot formation, where processes that affect soot formation can be more readily discerned. Soot formation pathways under such conditions are fraught with uncertainties, and soot models significantly overpredict polyaromatic hydrocarbon (PAH) and soot, so experimental data at these conditions will provide much needed data for improvements to PAH and soot models.

02 PETROLEUM↗

DOE OSTI2016

Lithium Ion Batteries in Electric Drive Vehicles

This research focuses on the technical issues that are critical to the adoption of high-energy-producing lithium Ion batteries. In addition to high energy density / high power density, this publication considers performance requirements that are necessary to assure lithium ion technology as the battery format of choice for electrified vehicles. Presentation of prime topics includes: long calendar life (greater than 10 years); sufficient cycle life; reliable operation under hot and cold temperatures; safe performance under extreme conditions; end-of-life recycling. To achieve aggressive fuel economy standards, carmakers are developing technologies to reduce fuel consumption, including hybridization and electrification. Cost and affordability factors will be determined by these relevant technical issues which will provide for the successful implementation of lithium ion batteries for application in future generations of electrified vehicles.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2013

Properties measurements of (U{sub 0.7}Pu{sub 0.3})O{sub 2-x} in PO{sub 2}-controlled atmosphere

The investigation of physical properties of uranium and plutonium mixed oxide (MOX) fuels is important for the development of fast reactor fuels. It is well known that MOX is a nonstoichiometric oxide, and the physical properties change drastically with the Oxygen-to-Metal (O/M) ratio. A control technique for O/M ratio was established for measurements of high temperature properties of uranium and plutonium mixed oxide fuels. Sintering behavior, thermal expansion and O/M change of (U{sub 0.7}Pu{sub 0.3})O{sub 2.00} and (U{sub 0.7}Pu{sub 0.3})O{sub 1.99} were investigated in PO{sub 2}-controlled atmosphere which was controlled by H{sub 2}/H{sub 2}O gas system. Sintering behavior changed drastically with O/M ratio, and shrinkage of (U{sub 0.7}Pu{sub 0.3})O{sub 2.00} was faster and more advanced at lower temperatures as compared with (U{sub 0.7}Pu{sub 0.3})O{sub 1.99}. Thermal expansion was observed to be slightly increased with decreasing O/M ratio. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2017

Development and Assessment of CTFFuel

This milestone report documents an approach that seeks to develop a standalone fuel solver to simulate steady-state and transient thermo-mechanical responses of light-water reactor fuel rods and assess its temperature predictions against analytical solutions, and a well-known and validated fuel performance code. This manuscript focuses on five major topics: (1) development of the CTFFuel, (2) discussion of the newly implemented fuel deformation models in dynamic gap conductance model of CTFFuel, (3) enabling the dynamic gap conductance model in VERA-CS, (4) verification of the solid conduction solution and comparison of the CTFFuel with respect to the workhorse code, CTF, and (5) benchmark of the thermal conductivity degradation using the burnup dependent fuel thermal conductivity models and benchmark of the fuel centerline temperature using the dynamic gap conductance model with Halden measurements and FRAPCON-4.0 simulation results. CTFFuel temperature predictions are compared to predictions from FRAPCON-4.0 for UO 2 , UO 2 +Gd 2 O 3 and MOX fuels through reactor’s life. The main motivation is to understand discrepancies between CTFFuel and FRAPCON-4.0’s temperature predictions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Benchmark Study on Innovative Fuels for Fast Reactors with fuel performance codes

The Working Party on the Scientific Issues of the Fuel Cycle (WPFC) has been established under the auspices of the Nuclear Energy Agency (NEA) Nuclear Science Committee (NSC), to co-ordinate scientific activities regarding various existing and advanced nuclear fuel cycles, including advanced reactor systems, associated chemistry and flowsheets, development and performance of fuels and materials, accelerators and spallation targets. Various expert groups were established to cover the above-mentioned topics. Within the WPFC, the Expert Group on Innovative Fuels (EGIF) was created with the objective of conducting joint and comparative studies to support the development of innovative fuels such as homogeneous and heterogeneous fuels, ADS fuels, and oxide, metal, nitride and carbide fuels, all of which can be implemented in advanced nuclear fuel cycles with fast reactors. The scope of the expert group covers innovative fuel fabrication techniques, irradiation performance of innovative fuels, characterisation and post-irradiation examination methods and predictive codes for innovative fuel fabrication and performance. This report presents the results of a benchmark study on innovative fuels for fast reactors using fuel performance codes. Irradiation results were shared among participants, and code calculations were performed to gain further insights on the fuel behaviour. Each participating institution used its own fuel performance code. Code to code and code to experiment comparisons are expected to provide data and improve understanding on the effects of minor actinides on fuel behaviour. In conclusion, the need for improvement of codes will be evaluated and the needs for new experimental data will be identified in order to finalise the code validation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2015

AREVA Team Enhanced Accident Tolerant Fuels Concepts (Phase 1A Final Report)

In response to the Department of Energy (DOE) funded initiative to develop and deploy lead fuel assemblies (LFAs) of Enhanced Accident Tolerant Fuel (EATF) into a US reactor within 10 years, AREVA put together a team to develop promising technologies for improved fuel performance during off normal operations. This team consisted of the University of Florida (UF) and the University of Wisconsin (UW), Savannah River National Laboratory (SRNL), Duke Energy and Tennessee Valley Authority (TVA). This team brought broad experience and expertise to bear on EATF development. AREVA has been designing; manufacturing and testing nuclear fuel for over 50 years and is one of the 3 large international companies supplying fuel to the nuclear industry. The university and National Laboratory team members brought expertise in nuclear fuel concepts and materials development. Duke and TVA brought practical utility operating experience. This report documents the results from the initial “discovery phase” where the team explored options for EATF concepts that provide enhanced accident tolerance for both Design Basis (DB) and Beyond Design Basis Events (BDB). The main driver for the concepts under development were that they could be implemented in a 10 year time frame and be economically viable and acceptable to the nuclear fuel marketplace. The economics of fuel design make this DOE funded project very important to the nuclear industry. Even incremental changes to an existing fuel design can cost in the range of $100M to implement through to LFAs. If this money is invested evenly over 10 years then it can take the fuel vendor several decades after the start of the project to recover their initial investment and reach a breakeven point on the initial investment. Step or radical changes to a fuel assembly design can cost upwards of $500M and will take even longer for the fuel vendor to recover their investment. With the projected lifetimes of the current generation of nuclear power plants large scale investment by the fuel vendors is difficult to justify. Specific EATF enhancements considered by the AREVA team were; Improved performance in DB and BDB conditions; Reduced release to the environment in a catastrophic accident; Improved performance during normal operating conditions; Improved performance if US reactors start to load follow; Equal or improved economics of the fuel; and Improvements to the fuel behavior to support future transportation and storage of the used nuclear fuel (UNF). In pursuit of the above enhancements, EATF technology concepts that our team considered were; Additives to the fuel pellets which included; Chromia doping to increase fission gas retention. Chromia doping has the potential to improve load following characteristics, improve performance of the fuel pellet during clad failure, and potentially lock up cesium into the fuel matrix; Silicon Carbide (SiC) Fibers to improve thermal heat transfer in normal operating conditions which also improves margin in accident conditions and the potential to lock up iodine into the fuel matrix; Nano-diamond particles to enhance thermal conductivity; Coatings on the fuel cladding; and Nine coatings on the existing Zircaloy cladding to increase coping time and reduce clad oxidation and hydrogen generation during accident conditions, as well as reduce hydrogen pickup and mitigate hydride reorientation in the cladding. To facilitate the development process AREVA adopted a formal “Gate Review Process” (GR) that was used to review results and focus resources onto promising technologies to reduce costs and identify the technologies that would potentially be carried forward to LFAs within a 10 year period. During the initial discovery phase of the project AREVA took the decision to be relatively hands off and allow our university and National Laboratory partners to be free thinking and consider options that would not be constrained by preconceived ideas from the fuel vendor. To counter this and to keep the partners focused, the GR process was utilized. During this GR process each of the team members presented their findings to a board made up of technical experts from utilities, fuel manufacturing experts, fuel technical experts, and fuel research and development (R&D) experts. During the initial 2 years of the project there were several major accomplishments. These accomplishments, along with the implications for successfully implementing EATF, are; The experimental spark plasma sintering process (SPS) process was successfully used to produce fuel pellets containing either 10% SiC whiskers or nano-diamond particles. The ability to use this process enables the thermal margin enhancements of the fuel additives to be realized. Without the SPS process, the conventional process cannot support adding pellet additives in the required quantities; Coatings of Ti2AlC were successfully applied to Zircaloy-4 cladding. Testing of Ti2AlC coatings at Loss of Cooling Accident (LOCA) conditions showed reduced cladding oxidation compared to present un-coated Zircaloy-4 cladding. This achievement allows the presently used cladding system to be retained so that the 10 year schedule can be met. Having to implement a new cladding material will extend the development schedule beyond 10 years; Several documents were produced to support future development, testing, and licensing of EATF, including a design requirements traceability matrix, a draft business plan, a draft test plan, a draft regulatory plan, and the acceptance criteria for lead fuel assembly insertion into a commercial reactor. This preparatory work lays the foundation for ensuring the future development plans address all the areas required to test, license, and manufacture the new EATF; and In addition, the high velocity oxy-fuel and electrophoretic deposition (EPD) coating application processes were dropped from further consideration due to their inability to meet manufacturing criteria. This allows the resources to be focused on the most promising EATF concepts identified. Future development opportunities that were identified during this work include; The use of SiC or diamond requires that a new pellet production technique (Spark Plasma Sintering), be developed. This entails investment in developing, proving and implementing a new commercial pellet production process. Development of the process to apply thinner coatings is required; Coatings cannot be too “thick” or they will displace a significant volume of water in the core resulting in reduced thermal hydraulic characteristics; Application of the coating at high temperature can affect the Zircaloy substrate. This will require the development and implementation of a new cladding coating manufacturing process; and Replace the Cold Spray (CS) cladding coating application with the Physical Vapor Deposition (PVD) process to eliminate duplication of work and provide greater control over coating thicknesses. This can result in a reduction in the final cycle economic penalty of coatings.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Rapid Assessment of Autoignition Propensity in Novel Fuels and Blends

We developed a computational strategy to correlate bulk combustion metrics of novel fuels and blends in the low-temperature autoignition regime with measurements of key combustion intermediates in a small-volume, dilute, high-pressure reactor. We used neural net analysis of a large simulation dataset to obtain an approximate correlation and proposed experimental and computational steps needed to refine such a predictive correlation. We also designed and constructed a high-pressure laboratory apparatus to conduct the proposed measurements and demonstrated its performance on three canonical fuels: n-heptane, i-octane, and dimethyl ether.

10 SYNTHETIC FUELS↗

DOE OSTI2024

The quest for safer nuclear fuels

Here, to increase the safety and performance of nuclear reactors, researchers are working on developing ‘accident tolerant’ fuels. Ideally, these fuel pellets will be less susceptible to swelling and be more resistant to extreme heat. This led chemists to develop uranium dioxide (UO 2 ) doped with divalent elements, E 2+ . These dopants can introduce vacancies into the lattice that lead to larger grain sizes, which create longer pathways for fission gasses to migrate out of the grains. In undoped fuel, fission gas build-up at grain boundaries causes the fuel pellet to swell. Therefore, having larger grains that slow fission gas migration into grain boundaries is highly desired. Divalent Cr 2+ ions are a commonly explored dopant for UO 2 fuels. These materials have larger grain sizes while maintaining the dissolution kinetics of undoped UO 2 , making their long-term storage and disposal paths similarly safe. Atomistic models have suggested that Mn 2+ is a conceivable alternative doping material, with the potential to increase the sizes of grains even more than Cr 2+ dopants. As such, experimental studies are required to understand the physical chemistry and reactivity of these potential fuels.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2013

Quantity and management of spent fuel from prototype and research reactors in Germany

Within the scope of an R and D project (project identification number FKZ 02 S 8679) sponsored by BMBF (Federal Ministry of Education and Research), the current state of storage and management of fuel elements from prototype and research reactors was established, and an approach for their future storage/management was developed. The spent fuels from prototype and research reactors in Germany that require disposal were specified and were described in regard to their repository-relevant characteristics. As there are currently no casks licensed for disposal in Germany, descriptions of casks that were considered to be suitable were provided. Based on the information provided on the spent fuel from prototype and research reactors and the potential casks, a technical disposal concept was developed. In this context, concepts to integrate the spent fuel from prototype and research reactors into existing disposal concepts for spent fuel from German nuclear power plants and for waste from reprocessing were developed for salt and clay formations. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

Identification of Process Suitable Diluent

The Sigma Team for Minor Actinide Separation (STMAS) was formed within the USDOE Fuel Cycle Research and Development (FCRD) program in order to develop more efficient methods for the separation of americium and other minor actinides (MA) from used nuclear fuel. The development of processes for MA separations is driven by the potential benefits; reduced long-term radiotoxicty of waste placed in a geologic repository, reduced timeframe of waste storage, reduced repository heat load, the possibility of increased repository capacity, and increased utilization of energy potential of used nuclear fuel. The research conducted within the STMAS framework is focused upon the realization of significant simplifications to aqueous recycle processes proposed for MA separations. This report describes the research efforts focused upon the identification of a process suitable diluent for a flowsheet concept for the separation of MA which is based upon the dithiophosphinic acid (DPAH) extractants previously developed at the Idaho National Laboratory (INL).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Mechanical Properties of Irradiated U-10wt%Mo Alloy Degraded by Porosity Development

A plate-type nuclear fuel consisting of a solid monolithic foil of U-10wt%Mo is under development for use in the United States’ high performance research reactors. In support of developing this fuel, the fuel has been fabricated for the first time by a commercial fuel vendor and subsequently irradiated in a test reactor. This provides an opportunity to evaluate post-irradiation mechanical properties of commercially fabricated fuel. Four-point bend testing was conducted on the irradiated U-10Mo fuel and the data produced includes bending strength and Young’s modulus. Although the material behaves in a brittle manner due to the developed porosity, a general trend of strength and modulus reduction are found as fission density increases. The data produced is evaluated using both Weibull statistics and a modulus degradation model with recommendations provided.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗