Atomic-scale modeling of complex oxides and nuclear fuels [Slides]
Abstract not provided.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
SEARCH · Engineering Papers
Results for “materials and fuels complex”
Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.
First Principle based Thermal Conductivity Modeling of Metal Alloys with Applications on Uranium Alloys
Thermal conductivity is an important materials property related to heat transport, which is essential to many applications, ranging from thermoelectrics to nuclear reactor materials. High- quality thermal conductivity data is critical to these materials and their associated technologies, including the nuclear fuel materials like traditional oxide fuels and metallic uranium (U) fuels, e.g. U-Zr and U-Mo alloys. And thermal conductivity modeling is widely used to interpolate or extrapolate experimental data, to obtain high-quality thermal conductivity data over wide temperature and composition range, and to understand the impacts of different factors including defects and microstructures. However, a general thermal conductivity model for metal alloys which can work regrading different phase components is still missing. Also, for U alloys, a thermal conductivity model working with different phases is needed. Therefore, in this work, we developed thermal conductivity models for metal alloys, based on ab-initio calculations, semi-classical physics rules, and limited experimental data. The goals of these models are to help obtain high- quality thermal conductivity data within a little experimental input as possible, have models that are extendable to varying microstructures, including different types of irradiation effects, and provide mechanistic understanding of heat transfer in the modeled alloys. In this work, our model solves several challenges in the development. The DFT-BTE approach is applied to decrease the reliance on experimental data and make the model extendable to composition changes and defects. A practical and efficient way to combine the DFT inputs with physics rules is pointed out in this work too. A staged approach, which starts from simple cases of elemental metals, then extends to solid solutions, different compound phases, and multi-phase mixtures, is presented to work with the metal alloys in different phase components. Our models are demonstrated respectively on aU for elemental metal model, on U-Zr and U-Mo alloys in aU temperature range for multi-phase mixture model, on high-temperature U-Zr, U-Nb, and U-Mo alloys in the body-centered cubic phase for concentrated solid solution model, and on irradiated U-Mo alloys for irradiated metal alloy model. All models show great agreement with experimental data. In these demonstrations, our model shows its advantages compared to previous empirical fitting model. Our model requires fewer experimental data, due to the inputs from DFT. The quantitative insights into the different physical factors are provided in our model, as it incorporates the electron and phonon scattering mechanisms. Our model also can be extended to incorporate the contributions of point defects, grain boundaries, and noble gas bubbles, to integrate their effects on heat transfer. This model can serve as both a foundation for understanding the more complex thermal conductivity of realistic U alloy fuels and a useful tool to guide further modeling of thermal conductivity to aid materials and device design.
11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Multiscale Patterning from Competing Interactions and Length Scales
We live in an era of complexity marked by impressive new tools powering the scientific method to accelerate discovery, prediction, and control of increasingly complex systems. In common with many disciplines and societal challenges and opportunities, materials and condensed matter sciences are beneficiaries. The volume and fidelity of experimental, computational, and visualization data available, and tools to rapidly interpret them, are remarkable. Conceptual frameworks, including multiscale, multiphysics modeling of this complexity, are fueled by the data and, in turn, guide directions for future experimental and computational strategies. In this spirit, we discuss the importance of competing interactions, length scales, and constraints as pervasive sources of spatio-temporal complexity. We use representative examples drawn from materials and condensed matter, including the important role of elasticity in some technologically important quantum materials.
36 MATERIALS SCIENCE↗
Alternative Materials Literature Review: A Review of Alternative Materials for Xenon Capture in Comparison to AgZ-PAN
A collaborative literature review between Idaho National Laboratory (INL) and Pacific National Laboratory (PNNL) was conducted to research alternative metals/materials for xenon adsorption in gaseous effluents generated from used nuclear fuel (UNF) reprocessing. The review was conducted to research sorbents that could outperform silver mordenite (AgZ) at ambient temperature. The use of silver requires complex and expensive waste disposal processes due to it being an RCRA metal, therefore alternative materials need to be researched and evaluated. The report details two different types of sorbent material: alternative zeolite materials and non-zeolite-based materials (i.e., MOFs, COFs, etc.). This report documents a brief history of the materials, what testing has been conducted on them, and what results suggest the possibility of outperforming the silver-based materials. Sorbent performance characteristics such as durability, capacity, and operating temperatures were evaluated. The simplicity of the sorbents was also evaluated, meaning how they are acquired (synthesized vs. naturally abundant). Recommendations were made for the most promising sorbents based on available research in the subject area and these recommended sorbents will be tested in the upcoming fiscal year. The recommended sorbents that are zeolite based are CHA zeolites, ZIF-69, and Na-ETS-10. The recommended sorbents that are non-zeolite based are SBMOF-1 and CC3.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Alternative Materials Literature Review: A Review of Alternative Materials for Xenon Capture in Comparison to AgZ-PAN
A collaborative literature review between Idaho National Laboratory (INL) and Pacific National Laboratory (PNNL) was conducted to research alternative metals/materials for xenon adsorption in gaseous effluents generated from used nuclear fuel (UNF) reprocessing. The review was conducted to research sorbents that could outperform silver mordenite (AgZ) at ambient temperature. The use of silver requires complex and expensive waste disposal processes due to it being an RCRA metal, therefore alternative materials need to be researched and evaluated. The report details two different types of sorbent material: alternative zeolite materials and non-zeolite-based materials (i.e., MOFs, COFs, etc.). This report documents a brief history of the materials, what testing has been conducted on them, and what results suggest the possibility of outperforming the silver-based materials. Sorbent performance characteristics such as durability, capacity, and operating temperatures were evaluated. The simplicity of the sorbents was also evaluated, meaning how they are acquired (synthesized vs. naturally abundant). Recommendations were made for the most promising sorbents based on available research in the subject area and these recommended sorbents will be tested in the upcoming fiscal year. The recommended sorbents that are zeolite based are CHA zeolites, ZIF-69, and Na-ETS-10. The recommended sorbents that are non-zeolite based are SBMOF-1 and CC3.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Low-spin cobalt(ii) redox shuttle by isocyanide coordination
Coordination of the strong-field ligand 2,6-dimethylphenyl isocyanide (DMP-CN) to the Co(PY5Me 2 ) framework, where PY5Me 2 represents the pentadentate ligand 2,6-bis(1,1-bis(2-pyridyl)ethyl)pyridine, has resulted in a new low-spin Co(II) complex with a relatively low reorganization energy and fast electron-transfer kinetics compared to the prototypical cobalt tris-bipyridine redox shuttle, [Co(bpy) 3 ] 3+/2+ , where bpy represents 2,2'-bipyridine. Despite nearly 160 mV reduced regeneration driving force, the [Co(PY5Me 2 )(DMP-CN)]3+/2+ redox shuttle displayed an increased regeneration efficiency relative to [Co(bpy)3] 3+/2+ , however recombination losses hinder the performance as evidenced by a reduced recombination resistance. Finally, future directions point to low-spin Co(II) redox shuttles with more negative redox potentials to be paired with a dye or dye mixture that absorbs into the near infrared region.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Perovskite-Derived Cs 2 SnCl 6 –Silica Composites as Advanced Waste Forms for Chloride Salt Wastes
Advanced materials and processes are required to separate halides and fission products from complex salt waste streams associated with the chemical reprocessing of used nuclear fuels and molten salt reactor technologies for immobilization into chemically durable waste forms. Here, in this work, we explore an innovative concept using metal-halide perovskites as advanced host phases to incorporate Cs and Cl with very high waste loadings. Wet chemistry-synthesized Cs 2 SnCl 6 powders from CsCl salt solutions are successfully encapsulated into a silica matrix to form a composite using low-temperature spark plasma sintering with tunable Cs and Cl loadings up to 31 wt.% and 26 wt.%, respectively. Chemical durability testing of the composite waste forms by semi-dynamic leaching experiments demonstrates that incongruent leaching mechanism dominated. The metal-halide perovskite-silica composite waste forms display exceptional chemical durability with the long-term release rates of Cs and Cl comparable to or outperforming the state-of-the-art waste form materials but with significantly higher waste loadings. The scalable synthesis of the metal-halide perovskite from wet-chemistry processes opens up new opportunities in designing perovskite-glass composite waste forms for salt wastes with very high waste loadings and exceptional chemical durability for the sustainable development of advanced fuel cycles and next-generation reactor technologies.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Development of High Capacity Energy Storage Materials
Hydrogen fuel cells have the potential to offer energy and power density advantages over lithium ion batteries in automotive and portable power applications when paired with an appropriate hydrogen storage system. Development of the ideal hydrogen storage material has been immensely sought after but plagued by limitations present in each type of material. These limitations typically include nonidealistic operational temperatures, low capacities, excessive costs, lack of reversibility, or evolution of impurities which irreversibly damage fuel cell performance. Many complex metal hydrides possess suitable hydrogen capacities but unfortunately suffer from impurity release. In order to address this problem, our team has explored in-situ catalyst doping of alkali metal amides to demonstrate methodologies to reduce ammonia release. The incorporation of iridium metal in lithium amide significantly reduces the ammonia release and decomposes the ammonia to provide additional hydrogen. Furthermore, we demonstrate, for the first time, high resistance of low temperature fuel cells to ammonia in comparison with typical proton exchange membrane fuel cells. The utilization of these two approaches in tandem provides a novel pathway for the development and implementation of high capacity energy storage materials for fuel cell applications.
25 ENERGY STORAGE↗
Comparative Structural Rigidity Analysis of the NBSR DDE and the NBSR LEU Fuel Element
The National Bureau of Standards Reactor (NBSR) is a 20-MW heavy-water moderated and cooled, enriched-fuel, tank-type reactor located in the NIST Center for Neutron Research laboratory complex. NBSR is one of six U.S. high performance research reactors (USHPRR), including one critical facility, that actively collaborates with the National Nuclear Security Administration (NNSA) Material Management and Minimization (M3) Reactor Conversion Program to convert from the use of highly enriched uranium fuel to the use of low-enriched uranium (LEU, < 20 wt% U-235) fuel. On the LEU U-10Mo fuel qualification side, mini-plate and large-plate irradiations have been successfully performed, and more experiments are either ongoing or planned. As an additional experimental campaign to support licensing of the LEU fuel for the use in the NBSR, the NBSR Design Demonstration Element (DDE) will be a full-sized test element similar to the NBSR LEU fuel element and irradiated in a test reactor under conditions as prototypic of the NBSR LEU fuel element operating conditions as possible.
21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
Electrocatalysis of Oxygen Reduction Reaction in a Polymer Electrolyte Fuel Cell with a Covalent Framework of Iron Phthalocyanine Aerogel
Carbon aerogels have been studied in the context of fuel cell electrodes mainly as catalyst support materials due to their high surface area, porosity, and electrical conductivity. Recently, aerogels composed solely of inorganic molecular complexes have shown to be promising materials for the electrocatalysis of oxygen reduction reaction (ORR). These aerogels consist of atomically dispersed catalytic sites. Herein, we report on the synthesis and characterization of an aerogel-based catalyst: iron phthalocyanine aerogel. It was synthesized by coupling of ethynyl-terminated phthalocyanine monomers and then heat-treated at 800 °C to increase its electrical conductivity and catalytic activity. Further, the aerogels reported here were tested as catalysts for ORR in acidic conditions for the first time and found to have a ultra-high number of atomically dispersed catalytic sites (7.11 × 10 20 sites g –1 ) and very good catalytic activity (E onset = 0.9 V vs RHE and TOF = 9.2 × 10 –3 e – s –1 site –1 at 0.8 V vs RHE). The iron phthalocyanine aerogel was also studied in a proton exchange membrane fuel cell, reaching a peak power density of 292 mW cm –2 and an open circuit voltage of 0.83 V.
25 ENERGY STORAGE↗
Evaluation of the ring tension test (RTT) for robust determination of material strengths
The ring tension test (RTT) is an experimental method for determining mechanical behavior in a material’s circumferential or hoop direction. It is a crucial test for testing anisotropic materials with tube geometry, such as nuclear fuel cladding or irradiated pipes. Several RTT configurations exist, each with their own advantages and disadvantages. However, this test is significantly more complex than traditional tensile testing and can be especially sensitive to small differences and inconsistencies in the test setup and geometry, ultimately affecting the derived mechanical properties. Previous research has focused on method development, and little work has been done on understanding the subtle differences between an ideal test and experiments, specifically when the tests are performed on highly irradiated materials in hot cells. In this work, a finite element-based investigation of the RTT is conducted to fill this gap. The two most used test configurations are investigated, comparing their ability to determine accurate material strengths through plastic deformation. Several non-ideal conditions and uncontrollable effects which are likely to occur during experimental testing such as machining tolerances, variations of specimen geometry from nominal dimensions, rotation of specimens and fixturing, and other test setup discrepancies are studied. The sensitivity of measured strengths to these conditions is presented. A mechanics-based approach to describing and correcting raw data to determine actual strengths is also included for one of the configurations, resulting in a robust correction method with highly accurate material strength measurements. Finally, based on these analyses, the hemicylindrical mandrel configuration is recommended with a gauge region oriented at a 45° angle.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Mechanics of the Ring Tension Test (RTT): A Finite Element-based Investigation
The ring tension test (RTT) is an experimental method for determining mechanical behavior in a material’s circumferential or hoop direction. It is a crucial test for testing anisotropic materials with tube geometry, such as nuclear fuel cladding or irradiated pipes. Several RTT configurations exist, each with their own advantages and disadvantages. However, this test is significantly more complex than traditional tensile testing and can be especially sensitive to small differences and inconsistencies in the test setup and geometry, ultimately affecting the derived mechanical properties. Previous research has focused on method development, and little work has been done on understanding the subtle differences between an ideal test and experiments, specifically when the tests are performed on highly irradiated materials in hot cells. In this work, a finite element-based investigation of the RTT is conducted. Two promising test configurations are investigated, comparing their ability to determine accurate material strengths through plastic deformation. Several non-ideal conditions and uncontrollable effects which are likely to occur during experimental testing such as machining tolerances, variations of specimen geometry from nominal dimensions, rotation of specimens and fixturing, and other test setup discrepancies are studied. The sensitivity of measured strengths to these conditions is presented. A mechanics-based approach to describing and correcting raw data to determine actual strengths is also included for one of the configurations, resulting in a robust correction method with highly accurate material strength measurements. Based on these analyses, the hemicylindrical mandrel configuration is recommended with a gauge region oriented at a 45° angle.
22 GENERAL STUDIES OF NUCLEAR REACTORS↗
Privacy Preservation from High-Performance Computing to Autonomous Science [Industrial and Governmental Activities]
High-Performance Computing (HPC) and Leadership-Class Supercomputing are driving forces behind scientific advancements, enabling researchers to tackle complex challenges in physics, chemistry, biology, and engineering. These systems power vast simulations and data analyses, fueling discoveries in fields ranging from materials science to climate modeling. However, their use often involves processing sensitive data—such as proprietary industry simulations, biomedical records, and national security computations—posing significant privacy concerns. In conclusion, this issue is amplified in collaborative environments like Department of Energy (DOE) user facilities, where HPC resources are shared across institutions to foster innovation.
Kotevska, Olivera [Oak Ridge National Laboratory (↗
Opportunities and Challenges of Lignin Utilization
Lignin is the most abundant non-carbohydrate component of plant cell walls and the largest aromatic source on earth. It is gaining more attention due to its potentials for many industrial applications. Compared to the applications of carbohydrate components like cellulose and hemicellulose, the utilization of lignin is challenging due to its natural rigidity, heterogeneity, and complexity. On the other hand, the successful utilization of lignin can broaden the spectrum of renewable resources in producing chemicals, fuels, and materials. In addition, value-added lignin products can enhance the economic competitivity of many biofuels and biochemicals mainly produced from cellulose and hemicellulose. In the last few decades, there have been notable improvements in fundamental understandings of the plant cell wall, lignin chemistry, catalysis, and other engineering principles, as well as the development of diverse conversion and characterization technologies. Prior to the detailed discussions of recent lignin utilization strategies through decomposition approaches such as thermochemical, biological, photoelectrochemical and electrochemical depolymerization and material approaches including carbon materials, adsorbents, thermosets, thermoplastics, hydrogels and nanoparticles, this chapter briefly discusses the types of lignin and its potentials and limitations based on its characteristics and applied processes.
Geun yoo, Chang↗
Engineering defect energy landscape of CoCrFeNi high-entropy alloys by the introduction of additional dopants
The concept of high-entropy alloys (HEAs) focusing on tuning the overall chemical complexity represents a novel alloy design strategy. In contrast, alloying of a metallic matrix with minor doping elements with limited and localized tunability has been a common practice to improve material performance. Combining the idea of globally engineering defect energy landscape in HEAs and the localized doping strategy in dilute alloys, in this work, we explore doping effects of minor elements in a HEA matrix to further enhance the overall and localized chemical tunability, aiming to improve its irradiation resistance. Specifically, we study the influence of minor Al, Cu, Ti, and Pd substitutional doping elements on defect energetics in a CoCrFeNi model HEA based on density-functional theory (DFT) calculations. The DFT results indicate that the formation and migration energies of vacancies can be strongly influenced when a dopant is introduced at the first nearest neighbor shells around a vacancy. On the other hand, interstitial energetics are only slightly affected. Among the four elements, Ti and Pd generally decrease vacancy formation energies and increase vacancy migration energies more significantly than Al and Cu. The doping effects become more pronounced when the concentration of the substitutional dopants increases. Based on the energy distributions obtained from DFT, we build a kinetic Monte Carlo (kMC) model to assess the impact of dopants on vacancy-mediated diffusivity in the doped HEAs. Our results suggest that Ti and Pd can lower the tracer diffusivity in the considered HEAs and act as trapping sites, whereas Cu may enhance the atomic transport. This work indicates that substitutional doping in HEAs is an effective strategy in metallurgy to further tune the defect and transport properties of complex alloys.
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
Large-Scale, GPU-Enhanced DFTB Approaches for Probing Multi-Component Alloys
The major goals of the project are to develop and apply GPU-enhanced density functional theory tight binding (DFTB) calculations for efficient simulations of structural materials of alloy systems. The figure below depicts the GPU algorithmic developments on the left that will be carried out, and the solid-state structures on the right are representative of the complex alloys that can be computed with the GPU-enhanced DFTB approach. The methodology and tools developed in this project encompass accurate intermolecular potentials and GPU enhancements to the density functional tight binding (DFTB) approach for high-throughput ab initio molecular dynamics calculations of multi-component alloys at elevated temperatures. While classical molecular dynamics can handle hundreds of thousands of atoms, it cannot provide a first-principles based description of large, multi-component alloys at the predictive quantum level. At the other extreme, conventional Kohn-Sham DFT methods can probe the true quantum nature of chemical systems; however, these methods cannot tackle the large sizes relevant to these multi-component systems. The DFTB-based ab initio molecular dynamics approach (coupled with our in-house GPU capabilities for enhanced speed) used in this project provides a viable approach for probing these large systems at a quantum level of detail that is significantly faster than current first-principle methods Collectively, the capabilities developed in this project directly respond to DOE HBCU-OMI, AOI 2-1 initiatives by (1) enabling accurate and efficient predictions and (2) bringing a fundamental understanding of structural interactions in these complex systems at elevated temperatures.
20 FOSSIL-FUELED POWER PLANTS↗
3D printing of metal-based materials for renewable energy applications
Large-scale renewable energy must overcome conversion and storage challenges before it can replace fossil fuels due to its intermittent nature. However, current sustainable energy devices still suffer from high cost, low efficiency, and poor service life problems. Recently, porous metal-based materials have been widely used as desirable cross-functional platforms for electrochemical and photochemical energy systems for their unique electrical conductivity, catalytic activity, and chemical stability. To tailor the porosity length scale, ordering, and compositions, 3D printing has been applied as a disruptive manufacturing revolution to create complex architected components by directly joining sequential layers into designed structures. In conclusion, this article intends to summarize cutting-edge advances of metal-based materials for renewable energy devices (e.g., fuel cells, solar cells, supercapacitors, and batteries) over the past decade.
36 MATERIALS SCIENCE↗