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The Strategic Benefit of Self Shielded Boxes for Storage and Disposal of Metallic Uranic Material-18141

Sellafield Ltd, on behalf of the Nuclear Decommissioning Authority (NDA), is responsible for the management of a number of facilities whose inventories include a range of metallic uranic material. Additional fuel and fuel bearing materials exist in the NDA estate, some of which are similar to the Sellafield-managed inventory and others present different management challenges. Whilst UK Government policy directs that some of these materials are assets and are therefore managed with eventual future use in mind, there remains a large quantity of material, principally either out-of-scope for reprocessing or which derives from legacy facilities, which is likely to be disposed of to a future Geological Disposal Facility (GDF). The majority of this material is stored under wet conditions to facilitate dose shielding and heat dissipation and will therefore require removal from wet storage, consolidation and conditioning, prior to transfer to GDF. In order to accelerate high hazard and risk reduction by sooner retrieval of legacy material from wetted storage, one of the legacy storage facilities has led technical work to develop the design of Self Shielded Boxes (SSBs) and to substantiate their use for interim storage of the materials in question. Use of the SSBs would represent a change of strategy on the Sellafield Site: historically, timescales for retrieval of material have been reliant upon a waste treatment and storage/disposal route being available. SSBs provide the opportunity to retrieve uranic materials from aging legacy storage facilities for immediate buffer storage, by decoupling the timing of retrieval from the availability of an onward route. An understanding was required of the scope for defining optimal routes for each metallic uranic fuel and fuel bearing material group for safe transport and storage commensurate with current final disposal assumptions and risks, taking into account international best practice. A study is underway to understand options for transfer of material into SSBs, buffer/interim storage locations, treatment/conditioning processes and transport to the GDF. This work forms the basis of a prioritised road-map for the development of routes for study material groups aligned with ongoing and existing planned technical work, which is a pre-requisite to strategy development. The ultimate output of the study will be identification of full life cycle management strategies for metallic uranic material from an enterprise perspective. The combination of this strategic work and ongoing technical work will underpin a series of decisions to divert sub-groups of uranic material away from currently assumed baseline routes in support of earliest practicable hazard and risk reduction. Hence, each decision will reduce the scope of a placeholder future uranic fuel treatment capability, which will diminish the associated British Pound 1 bn capital cost. To date, a technical case for interim storage of uranic material in SSBs has been substantiated for around two thirds of the study materials. The requirement for a new strategy at Sellafield was driven by technical development of SSBs in response to the needs of one programme, but this prompted the study into the potential utilisation of SSBs in order to derive benefit for the wider enterprise and across the NDA estate. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Exploring the Use of Muon Momentum for Detection of Nuclear Material Within Shielded Spent Nuclear Fuel Dry Casks

The inspection of the storage containers that house used nuclear fuel is an important issue facing the nuclear industry; currently, there are limited options available to provide for even minimal inspections. During the long storage life of the fuel, intermediate handling and transportation activities may take place that can create concerns regarding fuel integrity (safety) and continuity of knowledge (safeguards and security). Accidents and natural disasters also contribute to this concern. The reliable and safe management of used nuclear fuel is among the critical tasks to be addressed for the advancement of fission-based nuclear energy in the United States and elsewhere. Since the early 1950's, when the first nuclear power plant began to produce electricity, approximately 65,000 metric tons of used nuclear fuel have been generated in the United States. The postponement of the opening of a permanent repository until 2048 will lead to increased used fuel accumulation at reactor sites. A rapid increase in storage installations with more than 9,000 casks storing {approx}420,000 assemblies is anticipated by 2050 even if no new nuclear power plants are built. After used nuclear fuel has been placed inside a cask, the cask is sealed, not allowing for visual inspection. Conventional methods, e.g., x-rays, are limited in that they cannot penetrate dense, well-shielded objects. More sophisticated techniques, such as penetrating neutrons or proton radiography, require the use of an expensive accelerator. Efforts by Ziock et al. using neutron and gamma-ray imagers concluded that '...the signatures are deemed insufficient to uniquely identify individual casks of the same type...'. It was found that the gamma-ray and neutron images were dominated by diffusion and thermalization effects resulting from the large amount of shielding. One promising mode of inspection would use cosmic-ray muons. These muons are naturally generated, are able to penetrate dense materials, and are incident from all directions above the horizon. Tomography performed using these muons could potentially provide efficient, inexpensive, remote assessment of used nuclear fuel. However, current muon applications are limited in that they have not included momentum measurement. If momentum measurement could be incorporated, that would represent a big step forward because it would allow more accurate estimation of the muon observables, e.g., scattering variance. This approach has the potential to reconstruct the contents of a cask with improved resolution and identify partial defects, fuel assemblies, and individual fuel rods.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Swift BAT Perspective on Non-Thermal Emission in HIFLUGCS Galaxy Clusters

The search for diffuse non-thermal, inverse Compton (IC) emission from galaxy clusters at hard X-ray energies has been underway for many years, with most detections being either of low significance or controversial. Until recently, comprehensive surveys of hard X-ray emission from clusters were not possible; instead, individually proposed-for. long observations would be collated from the archive. With the advent of the Swift BAT all sky survey, any c1u,;ter's emission above 14 keV can be probed with nearly uniform sensitivity. which is comparable to that of RXTE, Beppo-SAX, and Suzaku with the 58-month version of the survey. In this work. we search for non-thermal excess emission above the exponentially decreasing, high energy thermal emission in the flux-limited HIFLUGCS sample. The BAT emission from many of the detected clusters is marginally extended; we are able to extract the total flux for these clusters using fiducial models for their spatial extent. To account for thermal emission at BAT energies, XMM-Newton EPIC spectra are extracted from coincident spatial regions so that both the thermal and non-thermal spectral components can be determined simultaneou,;ly in joint fits. We find marginally significant IC components in 6 clusters, though after closer inspection and consideration of systematic errors we are unable to claim a clear detection in any of them. The spectra of all clusters are also summed to enhance a cumulative non-thermal signal not quite detectable in individual clusters. After constructing a model based on single temperature

Wik, Daniel R.↗

Mass Dependency of Isotope Fractionation of Gases Under Thermal Gradient and Its Possible Implications for Planetary Atmosphere Escaping Process

Physical processes that unmix elements/isotopes of gas molecules involve phase changes, diffusion (chemical or thermal), effusion and gravitational settling. Some of those play significant roles for the evolution of chemical and isotopic compositions of gases in planetary bodies which lead to better understanding of surface paleoclimatic conditions, e.g. gas bubbles in Antarctic ice, and planetary evolution, e.g. the solar-wind erosion induced gas escaping from exosphere on terrestrial planets.. A mass dependent relationship is always expected for the kinetic isotope fractionations during these simple physical processes, according to the kinetic theory of gases by Chapman, Enskog and others [3-5]. For O-bearing (O16, -O17, -O18) molecules the alpha O-17/ alpha O-18 is expected at 0.5 to 0.515, and for S-bearing (S32,-S33. -S34, -S36) molecules, the alpha S-33/ αlpha S-34 is expected at 0.5 to 0.508, where alpha is the isotope fractionation factor associated with unmixing processes. Thus, one isotope pair is generally proxied to yield all the information for the physical history of the gases. However, we recently] reported the violation of mass law for isotope fractionation among isotope pairs of multiple isotope system during gas diffusion or convection under thermal gradient (Thermal Gradient Induced Non-Mass Dependent effect, TGI-NMD). The mechanism(s) that is responsible to such striking observation remains unanswered. In our past studies, we investigated polyatomic molecules, O2 and SF6, and we suggested that nuclear spin effect could be responsible to the observed NMD effect in a way of changing diffusion coefficients of certain molecules, owing to the fact of negligible delta S-36 anomaly for SF6.. On the other hand, our results also showed that for both diffusion and convection under thermal gradient, this NMD effect is increased by lower gas pressure, bigger temperature gradient and lower average temperature, which indicate that the nuclear spin effect may not be the significant contributor as the energies involved in the hyperfine effect are much smaller than those with molecular collisions, especially under convective conditions.

Sun, Tao↗

Demonstration of Subscale Cermet Fuel Specimen Fabrication Approach Using Spark Plasma Sintering and Diffusion Bonding

Nuclear thermal propulsion (NTP) has the potential to expand the limits of human space exploration by enabling crewed missions to Mars and beyond. The viability of NTP hinges on the development of a robust nuclear fuel material that can perform in the harsh operating environment (> or = 2500K, reactive hydrogen) of a nuclear thermal rocket (NTR) engine. Efforts are ongoing to develop fuel material and to assemble fuel elements that will be stable during the service life of an NTR. Ceramic-metal (cermet) fuels are being actively pursued by NASA Marshall Space Flight Center (MSFC) due to their demonstrated high-temperature stability and hydrogen compatibility. Building on past cermet fuel development research, experiments were conducted to investigate a modern fabrication approach for cermet fuel elements. The experiments used consolidated tungsten (W)-60vol%zirconia (ZrO2) compacts that were formed via spark plasma sintering (SPS). The consolidated compacts were stacked and diffusion bonded to assess the integrity of the bond lines and internal cooling channel cladding. The assessment included hot hydrogen testing of the manufactured surrogate fuel and pure W for 45 minutes at 2500 K in the compact fuel element environmental test (CFEET) system. Performance of bonded W-ZrO2 rods was compared to bonded pure W rods to access bond line integrity and composite stability. Bonded surrogate fuels retained structural integrity throughout testing and incurred minimal mass loss.

Barnes, Marvin W.↗

Validation of Thermal Scattering Laws for Light Water at Elevated Temperatures with Diffusion Experiments

Light water is the most important neutron moderator in many reactor applications. Thermal neutron scattering kernels for H bound in H 2 O are represented by ENDF-format thermal scattering laws (TSLs) evaluated at discrete temperatures T . Nuclear data evaluations are conventionally validated utilizing a combination of critical benchmarks and experimental cross section data. Existing public critical benchmarks may be inadequate for testing water TSLs over the full range of T of interest in reactor applications, and experimental thermal scattering cross section data for water is sparse at elevated T . In this work, MC21 is used to simulate the decay of the equilibrium thermal neutron flux in light-water spheres of several radii. The fundamental-mode time eigenvalue $\mathcal{a}$ is calculated at 22 °C and 227 °C (at saturation pressure) for each sphere using three different H-H 2 O TSLs. Fitting $\mathcal{a}$ to a polynomial function of geometric buckling allows calculation of the thermal neutron diffusion length L . Extrapolation lengths are treated as a function of the transport mean free path and geometry. Experimental L data from 25 publications at 49 temperatures (from 10 °C to 295 °C), computed by several different time-dependent and space-dependent decay methods, is used to develop an empirical fit of L vs. T . The MC21-calculated L for the TSLs tested are within ±1% of the predicted values at 22 °C and 227 °C. This validation approach, which may be repeated at arbitrary T , constitutes an integral benchmark specific to and characterizing the detailed physics of the thermal scattering kernel applied.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Kinetic theory of dense-fluid mixtures. IV.

Kinetic prediction theory for viscosity, thermal conductivity and diffusivity of binary liquid mixtures composed of molecules interacting with square-well potential

VISCOUS FLUID↗

Advanced Simulation Aided Metallic Fuel Design

Nuclear engineering is reaching a domain space in which computational power and methods are starting to surpass the models that are used to simulate nuclear fuel rods. As these models are updated, simulations utilizing different compositions, operating conditions, fabrication techniques, and geometries can provide core designers with an important first step towards fuel qualification. Due to the cost associated with fuel irradiations, it can be expected that time and money spent building better fuel models may provide an attractive return during initial studies of advanced fuels, especially with regards to fuels beyond the extensively studied uranium oxide system. In general, the primary U.S. experience with irradiated fuel rods beyond traditional oxide fuel is with binary (U-Zr) and ternary (U-Pu-Zr) metal fuels. The bulk of the experimental data for metal fuels is obtained from rods irradiated in the EBR-II sodium fast reactor (SFR), thus many of the correlations developed for metal fuels comes from the post-irradiation (PIE) examination of EBR-II rods. One of the unique characteristics that set U-Pu-Zr fuels apart from traditional oxide fuels is the presence of different phases that develop in the fuel during irradiation. Each of these different phases has unique thermal, mechanical, and diffusive behavior. The transitions between these phases are not static as the initially homogenous zirconium diffuses towards the center and edge of the fuel rod, resulting in a low-Zr, high-U ring. Along with the differing material properties that occur in each phase, the increase in uranium corresponds to an increase in localized fission and power production. The direct coupling between the thermal and diffusion solves highlights one of the many examples of tightly coupled phenomenon that are present in nuclear fuel, and motivation for the development of codes that simultaneously solve each piece of physics in a fully-coupled manner.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Heat Diffusion in Gases, Including Effects of Chemical Reaction

The diffusion of heat through gases is treated where the coefficients of thermal conductivity and diffusivity are functions of temperature. The diffusivity is taken proportional to the integral of thermal conductivity, where the gas is ideal, and is considered constant over the temperature interval in which a chemical reaction occurs. The heat diffusion equation is then solved numerically for a semi-infinite gas medium with constant initial and boundary conditions. These solutions are in a dimensionless form applicable to gases in general, and they are used, along with measured shock velocity and heat flux through a shock reflecting surface, to evaluate the integral of thermal conductivity for air up to 5000 degrees Kelvin. This integral has the properties of a heat flux potential and replaces temperature as the dependent variable for problems of heat diffusion in media with variable coefficients. Examples are given in which the heat flux at the stagnation region of blunt hypersonic bodies is expressed in terms of this potential.

Hansen, C. Frederick↗

Synthesis, Processing, and Use of Isotopically Enriched Epitaxial Oxide Thin Films

Isotopic engineering has emerged as a key approach to study the nucleation, diffusion, phase transitions, and reactions of materials at an atomic level. It aims to uncover mass transport pathways, kinetics, and operational and failure mechanisms of functional materials and devices. Understanding these phenomena leads to deeper insights into important physical processes, such as the transport of ions in energy conversion and storage devices and the role of active sites and supports during heterogeneous catalytic reactions. Likewise, isotopic engineering is being pursued as a means of modifying functionality to enable future technological applications. In this Account, we summarize our recent work employing isotope labeling (e.g., 18 O 2 and 57 Fe) during thin film synthesis and postgrowth processing to reveal growth mechanisms, defect chemistry, and elemental diffusion under working and extreme conditions. Isotope-resolved analysis techniques with nanometer-scale spatial resolution, such as time-of-flight secondary ion mass spectrometry and atom probe tomography, facilitate the accurate quantification of isotopic placement and concentration in our well-defined heterostructures with precisely positioned, isotope-enriched layers. By measuring the nanometer-scale redistribution between natural abundance and isotopically enriched oxygen layers during the deposition of Fe 2 O 3 and Cr 2 O 3 by molecular beam epitaxy, we identified intermixing processes driven by surface adatoms occurring both at the film growth surface and within the first few layers below the surface. Further insights into synthesis mechanisms were gained by studying the tungsten oxide thin films grown by evaporating WO 3 powder in the presence of background 18 O 2 , revealing minimal incorporation of background oxygen during the film formation process. Thermal and radiation-enhanced diffusion in epitaxial Fe and Cr oxides were precisely tracked using 18 O and 57 Fe tracer layers incorporated into model epitaxial oxide thin films. This approach has allowed us to access thermal diffusion behavior at lower temperatures than previously measured, revealing a potential changeover in diffusion mechanism. Understanding radiation-enhanced diffusion in model oxides that represent the surface layers on the structural components of nuclear reactors informs our understanding of their corrosion behavior under irradiation. Isotopic labeling can also provide unique insights into the surface exchange reactions and defect chemistry of electrocatalysts. For instance, tracking the change in 18 O concentration at the surface of an epitaxial LaNiO 3 thin film after the electrocatalytic oxygen evolution reaction revealed the participation of lattice oxygen, confirming a hypothesis that had been proposed previously. Lastly, we highlight a new direction wherein we perform in situ processing studies utilizing isotopic tracers in conjunction with model epitaxial thin films within the atom probe tomography instrument. Additionally, this Account illustrates the great potential of isotopic engineering to enable fundamental mechanistic insights into physical processes and engineer functional properties in epitaxial films, heterostructures, and superlattices.

36 MATERIALS SCIENCE↗

Atomistic modeling of metal–nonmetal interphase boundary diffusion

Atomistic computer simulations are applied to investigate the atomic structure, thermal stability, and diffusion processes in Al–Si interphase boundaries as a prototype of metal–ceramic interfaces in composite materials. Some of the most stable orientation relationships between the phases found in this work were previously observed in epitaxy experiments. Here, a non-equilibrium interface can transform to a more stable state by a mechanism that we call interface-induced recrystallization. Diffusion of both Al and Si atoms in stable Al–Si interfaces is surprisingly slow compared with diffusion of both elements in Al grain boundaries but can be accelerated in the presence of interface disconnections. A qualitative explanation of the sluggish interphase boundary diffusion is proposed. Atomic mechanisms of interphase boundary diffusion are similar to those in metallic grain boundaries and are dominated by correlated atomic rearrangements in the form of strings and rings of collectively moving atoms.

36 MATERIALS SCIENCE↗

Use of Diffusion Bonded Cu Strap and Integrated MLI for Thermal Control of 100 K IR Detector on L’Ralph Instrument

Passive cooling of cryogenic instruments is one of the most challenging aspects of spaceflight thermal control systems. They are highly sensitive to parasitic heat leaks from their warmer environment, especially the spacecraft components. The L’Ralph instrument on the Lucy mission is an example of such a system, with its LEISA detector requiring passive cooling to temperatures below 112 K. MLI performance can be measured in terms of estar, and analysts apply bias between a high and low estar value. This approach works well for conventional MLI at room temperature, however, it can be dangerous when a mission goes through a wide range of temperatures during its lifetime, with estar values increasing exponentially as temperatures get colder. Various estar correlations are presented as well as how L’Ralph is approaching the MLI problem with the use of IMLI. IMLI uses discrete spacers to isolate each layer, and doesn’t require intermediate layers such as dacron netting. This results in estar performance that can be more precisely estimated, and yields valuesaround 0.004 at the 112K operating temperature. L’Ralph is using IMLI on the backside of the radiator, which permits a more effective use of increased radiator area, by minimizing the area dependent heat leak impact from the instrument backloading. The detector is thermally coupled to the radiator via a diffusion bonded Cu strap. The diffusion bonding process chemically bonds the Cu foil ends in order to maximize heat transfer effectiveness across the multiple foils used. Employing a pressure compensation design via the use of Ti blocks and a clamp at the strap ends ensures that as temperatures go colder, pre-load is maintained in order to minimize resistance at the strap ends. The use of both of these technologies, and how they work together are crucial to the success of the L’Ralph thermal control system.

Thermal↗

Microstructural Analysis and Transport Properties of Thermally Sprayed Multiple-Layer Ceramic Coatings

In this paper, multilayer, graded ceramic/metal coatings were prepared by an air plasma spray method on Ti-6Al-4V, 4140 steel and graphite substrates. The coatings were designed to provide thermal barriers for diesel engine pistons to operate at higher temperatures with improved thermal efficiency and cleaner emissions. A systematic, progressive variation in the mixture of yttria-stabilized zirconia and bondcoat alloys (NiCoCrAlYHfSi) was designed to provide better thermal expansion match with the substrate and to improve thermal shock resistance and cycle life. Heat transfer through the layers was evaluated by a flash diffusivity technique based on a model of one-dimensional heat flow. The aging effect of the as-sprayed coatings was captured during diffusivity measurements, which included one heating and cooling cycle. The hysteresis of thermal diffusivity due to aging was not observed after 100-h annealing at 800 °C. The measurements of coatings on substrate and freestanding coatings allowed the influence of interface resistance to be evaluated. Finally, the microstructure of the multilayer coating was examined using scanning electron microscope and electron probe microanalysis.

36 MATERIALS SCIENCE↗

Diurnal variations in the thermosphere. II - Temperature, composition, and winds

The fundamental diurnal component of temperature, composition and wind fields is discussed for the thermosphere, the results delineated in terms of energy sources in the lower atmosphere, mesosphere and thermosphere, illustrating their relative significance. The diurnal component in the composition of H, He, O, O2 and Ar has been analyzed in terms of effects from thermal expansion in diffusive equilibrium and transport processes associated with chemistry, wind circulation, exospheric flow and escape. Next to thermal expansion, wind-induced diffusion is the single most important process; it dominates the diurnal variations of He and prevails in the variations of O, O2 and Ar below 200 km.

Mayr, H. G.↗

Numerical results for the thermal scattering functions

A recent formulation in radiative transfer defined the thermal scattering functions that characterize radiative transfer from a general plane-parallel finite medium driven solely by an internal distribution of thermal sources. Exiting diffuse intensities are expressed as space convolutions of the thermal scattering functions with any thermal source distribution. A parametric study is presented to obtain the basic structure of these scattering functions. The independent variables of these azimuthally independent functions are the direction cosine and source location, while the parameters are the single-scattering albedo, total optical depth, and the asymmetry factor in the Henyey-Greenstein phase function. The basic functional trends are discussed by using various parametric plots, and selected results are given to allow numerical checks. The computational method is invariant imbedding.

Cogley, A. C.↗