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DOE OSTI2023

High-temperature chromium diffusion in austenitic stainless steel: Ab initio molecular dynamics simulations

Chromium self-diffusion through stainless steel (SS) matrix and along grain boundaries is an important mechanism controlling SS structural materials corrosion. For this work, Cr diffusion in austenitic SS was simulated using canonical ab initio molecular dynamics with realistic models of type-316 SS bulk, with and without Cr vacancies, and a low-energy Σ3 twin boundary typically observed at active corrosion sites. Cr self-diffusion coefficients at 750 and 850 °C calculated using Einstein’s diffusion equation are 4.2 × 10 –6 and 8.1 × 10 –6 Å 2 ps –1 in pristine bulk, 3.8 × 10 –3 and 5.5 × 10 –3 Å 2 ps –1 in bulk including Cr vacancies, and 9.5 × 10 –2 and 1.0 × 10 –1 Å 2 ps –1 at a Σ3[1 1 1]60° twin boundary.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Microstructure and oxidation behavior of high strength steel AISI 410 implanted with nitrogen ion

Surface treatment by implantation with nitrogen-ion was performed on the commercial feritic high strength steel AISI 410 which is termed for high temperature applications. The aim of this research was focused on the surface modification to improve its high temperature oxidation property in the early stages. Ion implantation was carried out at acceleration energy of 100 KeV and ion current 10 mA for 30, 60 and 90 minutes. The samples were subjected to the high temperature oxidation test by means of thermogravimetry in a magnetic suspension balance (MSB) at 500 °C for 5 hours. The scanning electron microscopy (SEM), X-ray diffraction spectrometry (XRD) and Vickers Hardness measurement were used for sample characterization. The formation of ferro-nitride phase after implantation did not occur, however a thin layer considered to contain nitrogen interstitials was detected. The oxidation of both samples before and after implantation followed parabolic kinetics indicating inward growth of oxide scale characteristically due to diffusion of oxygen anions towards matrix surface. After oxidation test relativelly stable oxide scales were observed. Oxidation rates decreased proportionally with the increasing of implantation time due to the formation of oxide layer which is considered to be effectiv inhibitor for the oxygen diffusion.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Immobile Pore-Water Storage Enhancement and Retardation of Gas Transport in Fractured Rock

The effect of immobile pore-water on gas transport in fractured rock has implications for numerical modeling of soil vapor extraction, methane leakage, gaseous CO 2 leakage from sequestration operations, radionuclide transport from underground nuclear explosions, and nuclear waste disposal. While the ability for immobile pore-water storage to effect gas transport has been recognized in the past, the details and specific scenarios leading to enhanced, retarded, or unaffected gas transport have not been explored. In this paper, we performed numerical investigations into the enhancement and retardation of gas transport due to immobile pore-water storage in order to identify implications for gas transport applications. To do this, we developed a numerical approach to model gas transport with a single-phase flow solution coupled to the advection–dispersion equation modified to account for immobile pore-water storage. Other than the immobility of pore water, the formulation contains all other physics included in two-phase formulations (advective and diffusive gas transport in fractures and rock matrix and dissolution in immobile pore water). The assumption of immobile pore water is valid here since for many applications involving transport of soluble gases in fractured rock, the rate of aqueous transport is insignificant compared to gas transport. We verify our modeling approach with analytical solutions of: (1) 1D gas diffusion, (2) 1D gas advection, (3) barometric pumping of a fracture, and (4) gas transport with uniform fracture flow and diffusion into the matrix. We account for pore-water storage in our model by implementing a kinetic formulation of gas dissolution wherein the dissolved (aqueous) phase is considered an immobile constituent. Using this formulation, we model the effect of dissolution rate and saturation on the retardation of gas transport during pure diffusion and pure advection. We also demonstrate that although it is commonly believed that pore-water storage will always enhance gas transport in fractures during oscillatory flow (e.g., during reversing pressure gradients such as barometric pumping cycles), our simulations indicate that this may not always be the case. Our numerical investigations indicate that scenarios with lower effective diffusion coefficients ( ⪅ 10 − 5  m 2 / s ) and lower dissolution coefficients (i.e., the dissolution diffusion coefficient) ( ⪅ 10 − 11  m 2 / s ) will result in enhanced gas transport. Other combinations of gaseous diffusion and dissolution coefficients result in delayed gas transport or insignificant effect on gas transport. Based on these results, and given the fact that the free-air diffusion coefficients for many gases are slightly above 10 − 5  m 2 / s (near the boundary of enhanced/non-enhanced gas transport), tortuosity would have to be significant for gas transport enhancement to occur. Similarly, if we consider the free-water diffusion coefficient of gases (around 10 − 9  m 2 / s for many gases of interest) to be a maximum bound for the effective dissolution coefficients (i.e., the rate of diffusion into the water away from the air/water interface will limit the dissolution rate), the effective dissolution coefficient would have to be at least 2 orders of magnitude less for enhanced gas transport to occur. Otherwise, pore-water storage will delay or have negligible effect on the gas transport. The results also indicate that the assumption of instantaneous equilibrium, often invoked in numerical codes for dissolution processes (i.e., dissolution coefficient is effectively infinite), will fail to accurately capture important details of soluble gas transport. Finally, the implication of our results is that gas breakthrough times in fractured rock during oscillatory flow may be highly dependent on the effective gaseous diffusion and dissolution coefficients.

58 GEOSCIENCES↗

DOE OSTI2016

Implications of Grain-Scale Mineralogical Heterogeneity for Radionuclide Transport in Fractured Media

The geological disposal of nuclear waste is based on the multi-barrier concept, comprising various engineered and natural barriers, to confine the radioactive waste and isolate it from the biosphere. Some of the planned repositories for high-level nuclear waste will be hosted in fractured crystalline rock formations. The potential of these formations to act as natural transport barriers is related to two coupled processes: diffusion into the rock matrix and sorption onto the mineral surfaces available in the rock matrix. Different in situ and laboratory experiments have pointed out the ubiquitous heterogeneous nature of the rock matrix: mineral surfaces and pore space are distributed in complex microstructures and their distribution is far from being homogeneous (as typically assumed by Darcy-scale coarse reactive transport models). We use a synthetically generated fracture–matrix system to assess the implications of grain-scale physical and mineralogical heterogeneity on cesium transport and retention. The resulting grain-scale reactive transport model is solved using high-performance computing technologies, and the results are compared with those derived from two alternative models, denoted as upscaled models, where mineral abundance is averaged over the matrix volume. In the grain-scale model, the penetration of cesium into the matrix is faster and the penetration front is uneven and finger-shaped. The analysis of the cesium breakthrough curves computed at two different points in the fracture shows that the upscaled models provide later first-arrival time estimates compared to the grain-scale model. The breakthrough curves computed with the three models converge at late times. These results suggest that spatially averaged upscaled parameters of sorption site distribution can be used to predict the late-time behavior of breakthrough curves but could be inadequate to simulate the early behavior.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Unravelling the origins of shale nanoporosity using small-angle neutron scattering (SANS)

Hydrocarbon production from tight rocks is constrained by slow diffusion within the shale matrix, limited by small pore sizes and low permeability. The nanopore proportion and size distribution significantly influence matrix permeability, a key property for optimizing hydrocarbon recovery and supporting hydrogen production while minimizing environmental impacts. Small-angle neutron scattering (SANS) has been an important tool for exploring the characteristics and structure of shale nanopores. This study used SANS to analyze nanoporosity and pore size distribution (<100 nm) in tight rocks with varying compositions to determine the influence of rock heterogeneity on SANS measurements. Results showed that nanoporosity correlates with clay content, with the highest clay-rich shale (52.48 wt% clay) exhibiting 8.8 % nanoporosity. SANS also revealed more nanopores than traditional nitrogen adsorption measurements, affirming its ability to reflect bulk mineralogy and upholding the relevance of experimental findings using this technique to optimize field operational approaches.

03 NATURAL GAS↗

DOE OSTI2016

Aerosol detection efficiency in inductively coupled plasma mass spectrometry

We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10 -5 to 10 -11 . Free molecular heat and mass transfer theory was applied, but evaporative phenomena were not sufficient to explain the dependence of aerosol detection on particle diameter. Additional work is needed to correlate experimental data with theory for metal-oxides where thermodynamic property data are sparse relative to pure elements. Finally, when matrix effects and the diffusion of ions inside the plasma were considered, mass loading was concluded to have had an effect on the dependence of detection efficiency on particle diameter.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2018

Simulation of Nonequilibrium Dynamics on a Quantum Computer

We present a hybrid quantum-classical algorithm for the time evolution of out-of-equilibrium thermal states. Here, the method depends on classically computing a sparse approximation to the density matrix and, then, time-evolving each matrix element via the quantum computer. For this exploratory study, we investigate a time-dependent Ising model with five spins on the Rigetti Forest quantum virtual machine and a one spin system on the Rigetti 8Q-Agave quantum processor.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2018

Developing a Novel Hydrogen Sponge with Ideal Binding Energy and High Surface Area for Practical Hydrogen Storage

This Phase I (5 quarters) research project was to examine the validity of a new class of boron-containing polymer (B-polymer) frameworks, serving as the adsorbents for the practical onboard H2 storage applications. Three B-polymer frameworks were synthesized and investigated, which include B-poly(butyenylstyrene) (B-PBS) framework (A), B-poly(phenyldiacetyene) (B-PPDA) framework (B), and B-poly(phenyltriacetylene) (B-PPTA) framework (C). They are 2-D polymer structures with the repeating cyclic units that spontaneously form open morphology and the B-doped (p-type) π-electrons delocalized surfaces. The ideal B-polymer framework shall exhibit open micropores (pore size in the range of 1-1.5nm) with high surface area (>3000 m 2 /g), and the B-dopants in the conjugated framework shall provide high surface energy for interacting with H 2 molecules (an ideal H 2 binding energy in the range of 15-25 kJ/mol). The pore size distribution and H2 binding energy were investigated at both Penn State and NREL laboratories. So far, the experimental results show the successful synthesis of B-polymer frameworks with the relatively well-defined planar (2-D) structures. The intrinsically formed porous morphology exhibits a broad pore size distribution (in the range of 0.5-10 nm) with specific surface area (~1000 m 2 /g). The miss-alignment between 2-D layers may block some micropore channels and limit gas diffusion throughout the entire matrix. In addition, the 2-D planar conjugated structure may also allow free π-electrons delocalization throughout the framework, which significantly reduces the acidity of B-moieties (electron-deficiency).The resulting 2-D B-polymer frameworks only exhibit a small increase of H 2 binding energy in the range of 8-9 KJ/mole (quite constant over the whole sorption range).

08 HYDROGEN↗

DOE OSTI2026

Impact of Annealing on Superconducting Properties of Tantalum Thin Films

The pursuit for higher-coherence superconducting qubits has led to the adoption of new materials and innovative fabrication techniques. Among the commonly used superconducting materials, tantalum-based or tantalum-capped superconducting qubits have demonstrated the longest lifetimes, outperforming niobium devices even in the presence of their native oxides. Given the losses introduced by the surface oxide, one method to further improve performance is to reduce or eliminate the native oxide on tantalum through UHV annealing. In this work, we examine the effect of dissolved oxygen as a function of annealing temperature on the superconducting properties of tantalum thin films. Dissolved oxygen is quantified using atom probe tomography (APT) and secondary ion mass spectrometry (TOF-SIMS) and correlated with electromagnetic transport measurements performed using a Physical Property Measurement System (PPMS). This study observes that annealing decomposes the native oxide and drives oxygen diffusion into the film matrix. Increasing oxygen content decreases the superconducting transition temperature (Tc) and the residual resistivity ratio (RRR). The critical field decreases with the incorporation of oxygen, while the film’s coherence length decreases relatively by 5%. These results, as well as findings from ongoing studies linking fabrication processes to the structural and chemical properties of the superconducting film and Josephson junction, provide insight into effective strategies for improving the performance of superconducting devices.

Shinde, Maithilee [IIT, Chicago; Fermilab]↗

DOE OSTI2023

Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioning

Abstract. Evidence has accumulated that secondary organic aerosols (SOAs) exhibit complex morphologies with multiple phases that can adopt amorphous semisolid or glassy phase states. However, experimental analysis and numerical modeling on the formation and evolution of SOA still often employ equilibrium partitioning with an ideal mixing assumption in the particle phase. Here we apply the kinetic multilayer model of gas–particle partitioning (KM-GAP) to simulate condensation of semi-volatile species into a core–shell phase-separated particle to evaluate equilibration timescales of SOA partitioning. By varying bulk diffusivity and the activity coefficient of the condensing species in the shell, we probe the complex interplay of mass transfer kinetics and the thermodynamics of partitioning. We found that the interplay of non-ideality and phase state can impact SOA partitioning kinetics significantly. The effect of non-ideality on SOA partitioning is slight for liquid particles but becomes prominent in semisolid or solid particles. If the condensing species is miscible with a low activity coefficient in the viscous shell phase, the particle can reach equilibrium with the gas phase long before the dissolution of concentration gradients in the particle bulk. For the condensation of immiscible species with a high activity coefficient in the semisolid shell, the mass concentration in the shell may become higher or overshoot its equilibrium concentration due to slow bulk diffusion through the viscous shell for excess mass to be transferred to the core phase. Equilibration timescales are shorter for the condensation of lower-volatility species into semisolid shell; as the volatility increases, re-evaporation becomes significant as desorption is faster for volatile species than bulk diffusion in a semisolid matrix, leading to an increase in equilibration timescale. We also show that the equilibration timescale is longer in an open system relative to a closed system especially for partitioning of miscible species; hence, caution should be exercised when interpreting and extrapolating closed-system chamber experimental results to atmosphere conditions. Our results provide a possible explanation for discrepancies between experimental observations of fast particle–particle mixing and predictions of long mixing timescales in viscous particles and provide useful insights into description and treatment of SOA in aerosol models.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1989

Finite element modeling of frictionally restrained composite interfaces

The use of special interface finite elements to model frictional restraint in composite interfaces is described. These elements simulate Coulomb friction at the interface, and are incorporated into a standard finite element analysis of a two-dimensional isolated fiber pullout test. Various interfacial characteristics, such as the distribution of stresses at the interface, the extent of slip and delamination, load diffusion from fiber to matrix, and the amount of fiber extraction or depression are studied for different friction coefficients. The results are compared to those obtained analytically using a singular integral equation approach, and those obtained by assuming a constant interface shear strength. The usefulness of these elements in micromechanical modeling of fiber-reinforced composite materials is highlighted.

Ballarini, Roberto↗

NASA NTRS2007

Strengthening Aluminum Alloys for High Temperature Applications Using Nanoparticles of Al203 and Al3-X Compounds (X= Ti, V, Zr)

In this paper the effect of nanoparticles A12O3 and A13-X compounds (X= Ti, V, Zr) on the improvement of mechanical properties of aluminum alloys for elevated temperature applications is presented. These nanoparticles were selected based on their chemical stability and low diffusions rates in aluminum matrix at high temperatures. The strengthening mechanism for aluminum alloy is based on the mechanical blocking of dislocation movements by these nanoparticles. Samples were prepared from A12O3 nanoparticle preforms, which were produced using ceramic injection molding process and pressure infiltrated by molten aluminum. A12O3 nanoparticles can also be homogeneously mixed with aluminum powder and consolidated into samples through hot pressing and sintering. On the other hand, the Al3-X nanoparticles are produced as precipitates via in situ reactions with molten aluminum alloys using conventional casting techniques. The degree of alloy strengthening using nanoparticles will depend on the materials, particle size, shape, volume fraction, and mean inter-particle spacing.

Lee, Jonathan A.↗

DOE OSTI2023

Effective Lanthanide Diffusivity through U-Zr Metallic Fuel

Fuel-cladding chemical interaction (FCCI) is one of the main concerns for the performance of U-Zr metallic fuels. Although FCCI results in complex phase transformations and morphological changes in both the fuel and cladding sides of the interface, the formation of a brittle layer in the cladding side of the interface (sometimes referred to as wastage) has one of the most significant impacts on the cladding mechanical integrity. This brittle layer is associated with the formation of intermetallic compounds between the cladding constituents Fe, Cr and the lanthanide fission product species. The formation of this cladding wastage layer has been the focus of recent efforts to develop a mechanistic modeling framework, including production of lanthanides in the fuel, transport through the fuel to the fuel-cladding interface, and phase transformation to form intermetallic phases. To calculate the rate of transport of lanthanides through the fuel, a multi-scale computational approach has been used. Atomistic calculations have been performed to determine the diffusivities of Nd, the most prevalent lanthanide species, through the solid fuel matrix and along pore surfaces. These diffusivities have been used as input parameters for a mesoscale model to determine an effective diffusion coefficient that accounts for the formation of porosity, its interconnection, and infiltration with bond sodium from the fuel-cladding gap. The effective diffusivity has been used in engineering-scale simulations using the BISON fuel performance code, and BISON simulations have been compared to representative validation cases from the EBR-II reactor.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2019

Multiscale Modeling of CO 2 Migration and Trapping in Fractured Reservoirs with Validation by Model Comparison and Real-Site Applications (Final Technical Report)

This report documents the accomplishments achieved during the project titled “Multiscale Modeling of CO 2 Migration and Trapping in Fractured Reservoirs with Validation by Model Comparison and Real-Site Applications” funded by the US Department of Energy, Office of Fossil Energy. The objectives of the project were to develop modeling capabilities for predicting CO 2 and brine migration in fractured reservoirs during geologic carbon storage and to investigate the feasibility of carbon storage in fractured reservoirs using the newly developed modeling capabilities. To achieve these objectives new mass transfer functions were developed to adapt existing dual-continuum approaches – a commonly used approach in hydrocarbon reservoir modeling – to the CO 2 -brine system. In the dual-continuum approach the undisturbed rock matrix and the fractures are modeled as two separate continua, which are coupled through mass exchange of CO 2 and brine between the two continua. Mass transfer functions represent the mass exchange between fractures and the rock matrix, without requiring highly resolved numerical grids of individual fractures, thus allowing large modeling domains relevant to geologic carbon storage questions (tens of meters to hundreds of kilometers). Mass transfer functions for the exchange of both free-phase CO 2 and brine between fractures and rock matrix were developed for both the injection phase and the post-injection phase. During the injection phase the fractures are filled with CO 2 , while the rock matrix is initially filled with brine. Therefore, a mass transfer function was developed that is based on vertical displacement of brine by CO 2 in the rock matrix due to gravitational forces. Once CO 2 injection ceases and CO 2 migrates away from the direct vicinity of the injection site, the fractures will begin to re-fill with brine, while the rock matrix will have high CO 2 saturations. For these conditions a mass transfer functions was developed that is based on spontaneous imbibition, as the pore spaces in the rock matrix are much smaller than in the fractures. For formations with low permeability or high capillary entry pressure of the rock matrix, free-phase CO 2 may not be able to enter the rock matrix. However, free-phase CO 2 at the interface between fractures and rock matrix can dissolve into brine resident in the rock matrix. Therefore, additional mass transfer functions were developed based on aqueous-phase diffusion of CO 2 through the rock matrix. These mass transfer functions are based on existing solutions for diffusion and were expanded to be applicable to a variety of block shapes relevant to dual-continuum modeling. Implementations of the newly developed mass transfer functions showed that they give accurate results when compared to highly resolved models. In addition to developing new transfer functions, a new vertically-integrated dual-continuum modeling framework was developed. This development takes advantage of fast vertical segregation of CO 2 and brine in the fractures due to the density difference between CO 2 and brine and the high permeability of the fractures. Therefore, a vertically-integrated vertical equilibrium model for the fractures is coupled with a vertically-distributed model for the rock matrix. The newly developed approach significantly reduces the computational effort, but is only accurate for fracture permeabilities of 100 mD or higher. Finally, the newly developed models were applied to real and hypothetical geologic carbon storage sites to investigate the feasibility of using fractured reservoirs for carbon storage. The general results were, that storage of CO 2 – both as free-phase and dissolved – is feasible, but that storage capacities are likely lower than in unfractured systems. While the high permeability of the fractures reduces the injection pressure (or permits higher injection rates), fast migration of CO 2 may limit the overall storage volume, because CO 2 may escape laterally with not enough of the rock matrix being swept for effective storage.

20 FOSSIL-FUELED POWER PLANTS↗

DOE OSTI2020

Diffusive hydrodynamics from integrability breaking

We describe here the crossover from generalized to conventional hydrodynamics in nearly integrable systems. Integrable systems have infinitely many conserved quantities, which spread ballistically, in general. When integrability is broken, only a few of these conserved quantities survive. The remaining conserved quantities are generically transported diffusively; we further derive a compact and general diffusion equation for these. The diffusion constant depends on the matrix elements of the integrability-breaking perturbation; for a certain class of integrability-breaking perturbations, including long-range interactions, the diffusion constant can be expressed entirely in terms of generalized hydrodynamic data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

One-Dimensional Anomalous Diffusion of Gold Nanoparticles in a Polymer Melt

We investigated the dynamics of polymer-grafted gold nanoparticles loaded into polymer melts using x-ray photon correlation spectroscopy. For low molecular weight host matrix polymer chains, normal isotropic diffusion of the gold nanoparticles is observed. For larger molecular weights, anomalous diffusion of the nanoparticles is observed that can be described by ballistic motion and generalized Levy walks, similar to those often used to discuss the dynamics of jammed systems. Under certain annealing conditions, the diffusion is one-dimensional and related to the direction of heat flow during annealing and is associated with an dynamic alignment of the host polymer chains. Molecular dynamics simulations of a single gold nanoparticle diffusing in a partially aligned polymer network semiquantitatively reproduce the experimental results to a remarkable degree. Here, the results help to showcase how nanoparticles can under certain circumstances move rapidly in polymer networks.

36 MATERIALS SCIENCE↗

NASA NTRS1981

The effect of thermal cycling to 1100 C on the alpha /Mo/ phase in directionally solidified gamma/gamma-prime-alpha alloys

Specimens of gamma/gamma-prime-alpha (Mo) eutectic alloy were thermally cycled or isothermally exposed at temperatures of 1075 to 1100 C. Transmission electron microscopy examination of cycled specimens indicated that even an exposure of 10 minutes effected noticeable changes in the shape of the alpha phase, and that the changes were cumulative as more cycles were added. The cross sections of fine, smooth fibers changed from rectangles to octagons, while lamellae and irregular shapes spheroidized. These effects are attributed to the differences in thermal expansion coefficients between the alpha phase and the gamma/gamma-prime matrix, and to the higher diffusion rates prevailing at elevated temperatures. Where the configuration of the alpha phase is a simple shape, such as a fiber, increasing the temperature eventually brings about a stress free interface between the alpha phase and the matrix by differential thermal expansion. Where the shape of the alpha phase is more complex, a stressed interface persists to higher temperatures where diffusion produces the more drastic morphological changes.

Harf, F. H.↗

DOE OSTI2017

Transport properties of C and O in UN fuels

Uranium nitride fuel is considered for fast reactors (GEN-IV generation and space reactors) and for light water reactors as a high-density fuel option. Despite this large interest, there is a lack of information about its behavior for in-pile and out-of-pile conditions. From the present literature, it is known that C and O impurities have significant influence on the fuel performance. Here we perform a systematic study of these impurities in the UN matrix using electronic-structure calculations of solute-defect interactions and microscopic jump frequencies. These quantities were calculated in the DFT + U approximation combined with the occupation matrix control scheme, to avoid convergence to metastable states for the 5f levels. The transport coefficients of the system were evaluated with the self-consistent mean-field theory. It is demonstrated that carbon and oxygen impurities have different diffusion properties in the UN matrix, with O atoms having a higher mobility, and C atoms showing a strong flux coupling anisotropy. The kinetic interplay between solutes and vacancies is expected to be the main cause for surface segregation, as incorporation energies show no strong thermodynamic segregation preference for (001) surfaces compared with the bulk.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗