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At least 1,333 records · Page 74

Effect of the Form of Iron on HLW Melt Rate

The primary objective of the work reported herein was to determine the effect of the form of iron in the HLW stream on feed processing rate. Secondary objectives were to determine the effect of iron form on feed properties, glass properties, and carryover from the melter during vitrification. This was accomplished by replacing the Fe(OH) 3 used in a previously tested simulant for C-106/AY-102 actual waste with either goethite (FeO(OH)), hematite (Fe 2 O 3 ), magnetite (Fe 3 O 4 ), or a mixture of iron oxides, and processing the resulting melter feeds on the DM100 melter system. Glass forming additives were combined with the high iron simulant to produce melter feed targeting the HLW-NG-Fe2 glass composition. Melter feed samples also underwent testing for rheological properties and processing rate using a VGF system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Does Explosive Nuclear Burning Occur in Tidal Disruption Events of White Dwarfs by Intermediate-mass Black Holes?

We investigate nucleosynthesis in tidal disruption events (TDEs) of white dwarfs (WDs) by intermediate-mass black holes. We consider various types of WDs with different masses and compositions by means of three-dimensional (3D) smoothed particle hydrodynamics (SPH) simulations. We model these WDs with different numbers of SPH particles, N , from a few 10{sup 4} to a few 10{sup 7} in order to check mass resolution convergence, where SPH simulations with N > 10{sup 7} (or a space resolution of several 10{sup 6} cm) have unprecedentedly high resolution in this kind of simulation. We find that nuclear reactions become less active with increasing N and that these nuclear reactions are excited by spurious heating due to low resolution. Moreover, we find no shock wave generation. In order to investigate the reason for the absence of a shock wave, we additionally perform one-dimensional (1D) SPH and mesh-based simulations with a space resolution ranging from 10{sup 4} to 10{sup 7} cm, using a characteristic flow structure extracted from the 3D SPH simulations. We find shock waves in these 1D high-resolution simulations, one of which triggers a detonation wave. However, we must be careful of the fact that, if the shock wave emerged in an outer region, it could not trigger the detonation wave due to low density. Note that the 1D initial conditions lack accuracy to precisely determine where a shock wave emerges. We need to perform 3D simulations with ≲10{sup 6} cm space resolution in order to conclude that WD TDEs become optical transients powered by radioactive nuclei.

79 ASTRONOMY AND ASTROPHYSICS↗

Fast predictions of liquid-phase acid-catalyzed reaction rates using molecular dynamics simulations and convolutional neural networks

The rates of liquid-phase, acid-catalyzed reactions relevant to the upgrading of biomass into high-value chemicals are highly sensitive to solvent composition and identifying suitable solvent mixtures is theoretically and experimentally challenging. We show that the complex atomistic configurations of reactant–solvent environments generated by classical molecular dynamics simulations can be exploited by 3D convolutional neural networks to enable accurate predictions of Brønsted acid-catalyzed reaction rates for model biomass compounds. We develop a 3D convolutional neural network, which we call SolventNet, and train it to predict acid-catalyzed reaction rates using experimental reaction data and corresponding molecular dynamics simulation data for seven biomass-derived oxygenates in water–cosolvent mixtures. We show that SolventNet can predict reaction rates for additional reactants and solvent systems an order of magnitude faster than prior simulation methods. This combination of machine learning with molecular dynamics enables the rapid, high-throughput screening of solvent systems and identification of improved biomass conversion conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interinstitutional Study of the New EURO-GANEX Process Resistance by Gamma Irradiation Test Loops

As part of the homogeneous actinides recycling strategy, the EURO-GANEX process is one of the most promising options to achieve the goal of minor actinides recovery. However, EURO-GANEX also has various drawbacks that are being addressed. Improvements made to EURO-GANEX system have resulted in the emergence of the so-called New EURO-GANEX process, where the composition of the solvent has been modified by replacing TODGA and DMDOHEMA with cis-mTDDGA in the organic phase and SO3-Ph-BTP with PyTri-Diol in the aqueous phase in order to resolve important issues. The objective of this work is twofold: evaluate the gamma radiolysis resistance of the new EURO-GANEX process by dynamic irradiation conditions simulating the three main steps of the process and validate the design of CIEMAT Náyade, CEA Marcel and INL irradiation loop devices since each of them mimics different aspects of the real process. Náyade and the INL loops could irradiate together the organic and aqueous phases, whereas in the CEA loop, the irradiated solvent is recycled continuously inside a platform with several stages of mixer-settlers containing aqueous flows simulating the three main steps of the process. The extraction performances and changes in the composition of the solvent have been analysed during the irradiation experiment by different techniques: gamma spectrometry and ICP-MS/OES for cations or tracers extraction, and HPLC-MS to quantify the degradation and evaluate the degradation compounds. Additionally, in spite of some differences between the three-irradiation facilities, this inter-institutional study shows that they are three comparative tools, which provide results on the stability towards radiolysis of a liquid-liquid extraction system. Favourable extraction results for the different steps are obtained according to the static irradiation studies found in literature. However, the degradation of cis-mTDDGA is appreciable leading to degradation compounds, some of which form precipitates and produce important changes in viscosity, important aspects that must be addressed prior to the successful industrial application of the new EURO-GANEX process.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE-GENIORS Dynamic Irradiation Testing

As part of the homogeneous actinides recycling strategy, the EURO-GANEX process is one of the most promising options to achieve the goal of minor actinides recovery. Improvements made to EURO-GANEX system have resulted in the emergence of the so-called New EURO-GANEX process, where the composition of the solvent has been modified by replacing TODGA and DMDOHEMA with cis-mTDDGA in the organic phase and SO3-Ph-BTP with PyTri-Diol in the aqueous phase in order to resolve important issues. The objective of this work is twofold: evaluate the gamma radiolytic resistance of the new EURO-GANEX process by dynamic irradiation conditions simulating the three main steps of the process, and validate the design of CIEMAT Náyade, CEA Marcel and INL irradiation loop devices since each of them mimics different aspects of the real process. Náyade and the INL loops could irradiate the organic and aqueous phases together, whereas in the CEA loop, the irradiated solvent is recycled continuously inside a platform with several stages of mixer-settlers containing aqueous flows simulating the three main steps of the process. The extraction performances and changes in the composition of the solvent have been analyzed during the irradiation experiment by different techniques: gamma spectrometry and ICP-MS/OES for cations or radioactive tracer extraction, and HPLC-MS to identify and quantify the degradation compounds. Despite some differences between the three-irradiation facilities, this inter-institutional study shows that these three comparative tools provide similar trends in the radiolytic stability of a liquid-liquid extraction system. Favourable extraction results for the different steps are obtained according to the static irradiation studies found in literature. However, the degradation of cis-mTDDGA is appreciable leading to degradation compounds, some of which form precipitates and produce important changes in viscosity, important aspects that must be addressed prior to the successful industrial application of the new EURO-GANEX process.

38 - RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCL↗

Field theoretic simulations of polymer nanocomposites

Polymer field theory has emerged as a powerful tool for describing the equilibrium phase behavior of complex polymer formulations, particularly when one is interested in the thermodynamics of dense polymer melts and solutions where the polymer chains can be accurately described using Gaussian models. However, there are many systems of interest where polymer field theory cannot be applied in such a straightforward manner, such as polymer nanocomposites. Current approaches for incorporating nanoparticles have been restricted to the mean-field level and often require approximations where it is unclear how to improve their accuracy. In this paper, we present a unified framework that enables the description of polymer nanocomposites using a field theoretic approach. This method enables straightforward simulations of the fully fluctuating field theory for polymer formulations containing spherical or anisotropic nanoparticles. We demonstrate our approach captures the correlations between particle positions, present results for spherical and cylindrical nanoparticles, and we explore the effect of the numerical parameters on the performance of our approach.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dislocation-graphene interactions in Cu/graphene composites and the effect of boundary conditions: a molecular dynamics study

Here, in this paper, systematic molecular dynamics simulations were employed to study dislocation-graphene interactions in Cu/graphene systems using two carefully selected configurations: (i) edge dislocations in the pileup interacting with graphene during nanoindentation and (ii) complex dislocations interacting with graphene in compression of layered nanopillars. The intrinsic and extrinsic size effects were investigated with respect to varying the Cu lamella thickness and pillar sizes, revealing an anomalous extrinsic size effect: the smaller, the weaker. To understand which boundary conditions are physically consistent, both free and periodic graphene were considered. It was seen that edge dislocations in the pileup continuously transmitted across the free graphene through Cu/graphene interfacial sliding and graphene reorientation, whereas transmission was very difficult for periodic graphene as its in-plane deformation was required. In compression of Cu/graphene nanopillars, the strengthening effect of free graphene was found to be less obvious than that of the periodic case, which could be attributed to free graphene edges acting as dislocation sources after the compressed Cu overflowed the graphene sheet from all directions. We therefore conclude that the strengthening effect of periodic graphene inclusions appears to be overestimated, such that free graphene should be more appropriate.

36 MATERIALS SCIENCE↗

Anatomy of Local Structural Disorder of Ni(II) Species in MgCl 2 –KCl Molten Salts

Understanding the speciation of metal ions dissolved in molten salts (MS) is critical for enabling a broad range of high-temperature energy applications, including MS nuclear reactors and concentrated solar power plants. However, due to the inherent dynamicity of metal species in the MS environment and the strong temperature dependencies of their multiple coexisting forms, they are difficult to resolve structurally. Herein, we show that combining in situ X-ray absorption spectroscopy (XAS) with ab initio molecular dynamics (AIMD) simulations is necessary to uncover and quantify the coexisting coordination states of Ni(II) in molten MgCl 2 –KCl mixtures and explain how the temperature and salt composition control their relative populations. Furthermore, from the interionic angle and distance distributions of nickel in different coordination states obtained from AIMD simulations, it is evident that for each coordination state, the width and skewness of their bonding distributions increase with increasing coordination number. In conclusion, the combination of XAS with first-principles modeling to resolve metastable metal species in MS is critical for understanding their behavior over a wide range of temperatures and chemical environments in nuclear and solar applications.

36 MATERIALS SCIENCE↗

Molecular dynamics studies of fundamental bulk properties of palladium hydrides for hydrogen storage

Solid-state hydrogen storage materials undergo complex phase transformations whose behavior are collectively determined by thermodynamic (e.g., Gibbs free energy), mechanical (e.g., lattice and elastic constants), and mass transport (e.g., diffusivity) properties. These properties depend on the reaction conditions and evolve continuously during (de)hydrogenation. Thus, they are difficult to measure in experiments. Because of this, past progress to improve solid-state hydrogen storage materials has been prolonged. Using PdH x as a representative example for interstitial metal hydride, we have recently applied molecular dynamics simulations to quantify hydrogen diffusion in the entire reaction space of temperature and composition. In this paper, we have further applied molecular dynamics simulations to obtain well-converged expressions for lattice constants, Gibbs free energies, and elastic constants of PdH x at various stages of the reaction. Finally, our studies confirm significant dependence of elastic constants on temperature and composition. Specifically, a new dynamic effect of hydrogen diffusion on elastic constants is discovered and discussed.

08 HYDROGEN↗

PERFORMANCE EVALUATION OF CEILING RADIANT COOLING SYSTEM IN COMPOSITE CLIMATE

Radiant cooling systems are proving to be an energy efficient solution due to higher thermal capacity of cooling fluid especially for the buildings that require individual zone controls and where the latent loads are moderate. The Conventional air conditioners work at very low temperature i.e.5-8 c (refrigerant evaporator inlet) while the radiant cooling systems, also referred as high temperature cooling system, work at high temperatures i.e. 14-18 c. The radiant cooling systems can maintain lower MRT (Mean Radiant Temperature) as ceiling panels maintain uniform temperature gradient inside room and provide higher human comfort. The radiant cooling systems are relatively new systems and their operation and energy savings potential are not quantified for a large number of buildings and operational parameters. Moreover, there are only limited numbers of whole building simulation studies have been carried out for these systems to have a full confidence in the capability of modelling tools to simulate these systems and predict the impact of various operating parameters. Theoretically, savings achieve due to higher temperature set point of chilled water, which reduces chiller-running time. However, conventional air conditioner runs continuously to maintain requisite temperature. In this paper, experimental study for performance evaluation of radiant cooling system carried out on system installed at Malaviya National Institute of Technology Jaipur. This paper quantifies the energy savings opportunities and effective temperature by radiant cooling system at different chilled water flow rates and temperature range. The data collected/ analysed through experimental study will used for calibration and validation of system model of building prepared in building performance simulation software. This validated model used for exploring optimized combinations of key parameters for composite climate. These optimized combinations will used in formulation of radiant cooling system operations control strategy.

Ceiling Panels↗

Physics-driven Explosions of Stripped High-mass Stars: Synthetic Light Curves and Spectra of Stripped-envelope Supernovae with Broad Light Curves

Stripped-envelope supernovae (SESNe) represent a significant fraction of core-collapse supernovae, arising from massive stars that have shed their hydrogen and, in some cases, helium envelopes. The origins and explosion mechanisms of SESNe remain a topic of active investigation. In this work, we employ radiative-transfer simulations to model the light curves and spectra of a set of explosions of single, solar-metallicity, massive Wolf–Rayet stars with ejecta masses ranging from 4 to 11 M ⊙ , which were computed from a turbulence-aided and neutrino-driven explosion mechanism. We analyze these synthetic observables to explore the impact of varying ejecta mass and helium content on observable features. We find that the light curve shape of these progenitors with high ejecta masses is consistent with observed SESNe with broad light curves but not the peak luminosities. The commonly used analytic formula based on rising bolometric light curves overestimates the ejecta mass of these high-initial-mass progenitor explosions by a factor of up to 2.6. In contrast, the calibrated method by Haynie et al., which relies on late-time decay tails, reduces uncertainties to an average of 20% within the calibrated ejecta mass range. Spectroscopically, the He I 1.083 μm line remains prominent even in models with as little as 0.02 M ⊙ of helium. However, the strength of the optical He I lines is not directly proportional to the helium mass but instead depends on a complex interplay of factors such as the 56 Ni distribution, composition, and radiation field. Thus, producing realistic helium features requires detailed radiative transfer simulations for each new hydrodynamic model.

79 ASTRONOMY AND ASTROPHYSICS↗

The influence of fusion-relevant D 2 -0.1He plasma on Be-W mixed-materials

We report compositionally homogeneous mixed-material layers of Be and W, ∼2 μm thick, and of various W contents (spanning 0–100 at.% W), are produced by thermionic vacuum arc deposition. The layers are exposed to low energy (∼50 eV), high ion flux (6–8 × 10 22 m −2 s −1 ) D 2 -0.1He (10% He) mixed species plasma at 473 K and 1073 K to simulate ITER-like first wall and divertor plasma-material interaction. Surface morphological and compositional analysis is conducted prior and subsequent to plasma exposure. The action of the plasma produces almost complete depletion of Be from the near surface, and this is found regardless of the exposure temperature or initial composition. In the exposure case of 473 K, thermal desorption spectrometry reveals decreased D retention in W rich compositions compared to similar exposure in D 2 plasma without He, but no discernable difference is noted in Be rich compositions. At 1073 K, surface enrichment in W, by depletion of the Be, results in He induced W “fuzz” structures for all Be-W compositions explored.

36 MATERIALS SCIENCE↗

Sensitivity of summer ensembles of fledgling superparameterized U.S. mesoscale convective systems to cloud resolving model microphysics and grid configuration

The sensitivities of simulated mesoscale convective systems (MCSs) in the central U.S. to microphysics and grid configuration are evaluated here in a global climate model (GCM) that also permits global-scale feedbacks and variability. Since conventional GCMs do not simulate MCSs, studying their sensitivities in a global framework useful for climate change simulations has not previously been possible. To date, MCS sensitivity experiments have relied on controlled cloud resolving model (CRM) studies with limited domains, which avoid internal variability and neglect feedbacks between local convection and larger-scale dynamics. However, recent work with superparameterized (SP) GCMs has shown that eastward propagating MCS-like events are captured when embedded CRMs replace convective parameterizations. This study uses a SP version of the Community Atmosphere Model version 5 (SP-CAM5) to evaluate MCS sensitivities, applying an objective empirical orthogonal function algorithm to identify MCS-like events, and harmonizing composite storms to account for seasonal and spatial heterogeneity. A five-summer control simulation is used to assess the magnitude of internal and interannual variability relative to 10 sensitivity experiments with varied CRM parameters, including ice fall speed, one-moment and two-moment microphysics, and grid spacing. MCS sensitivities were found to be subtle with respect to internal variability, and indicate that ensembles of over 100 storms may be necessary to detect robust differences in SP-GCMs. Furthermore, these results emphasize that the properties of MCSs can vary widely across individual events, and improving their representation in global simulations with significant internal variability may require comparison to long (multidecadal) time series of observed events rather than single season field campaigns.

54 ENVIRONMENTAL SCIENCES↗

Estimating the reaction parameters of oil shale pyrolysis and oil shale grade using temperature transient analysis and inverse modeling

Grade of oil shale and reaction parameters of in-situ pyrolysis must be identified for the prediction of productivity before actual heating and production. Identification of oil shale grade and reaction parameters depends on laboratory experiments on core samples. However, laboratory-determined parameters can be different from those representing in-situ reservoir conditions. We use inverse modeling to determine oil shale grade and reaction parameters. The inversions are based on a forward model that simulates heat injection into a well. Temperature at the heating well is affected by a thermal skin effect as a result of a decrease of composite thermal conductivity around the heater due to the decomposition-induced porosity increase. Synthetic observations of heater temperature are generated from a forward simulation. Temperature difference and its derivative are used in synthetic inversions to estimate oil shale grade and parameters of active decomposition reactions with an error below 1%. Finally, the proposed methodology of inverse modeling is expected to successfully estimate the oil shale grade and reaction parameters without core sampling and subsequent surface experiments.

04 OIL SHALES AND TAR SANDS↗

SAS4A/SASSYS-1 Code Improvements for FY2016

SAS4A/SASSYS-1 is a simulation tool used to perform deterministic analysis of anticipated events as well as design basis and beyond design basis accidents for advanced reactors. This report summarizes ongoing tasks to modernize the SAS4A/SASSYS-1 code system to improve internal data management, update several other code modules, and add new features. Code modernization activities focused on eliminating legacy data management in the balance-of-plant module, which was the only module that still used non-portable data allocation. Code extensions include the development of a new axial expansion model that can accurately account for non-uniform or heterogeneous fuel compositions. The most significant accomplishment is the addition of uncertainty quantification capabilities for transient simulations using the Dakota toolkit from Sandia National Laboratory. The motivation for performing these updates stems from the relevance of SAS4A/SASSYS-1 to a number of U.S. Department of Energy programs as well as domestic and international collaborations. External collaborations have also produced improvements in the SAS4A/SASSYS-1 code, and these are summarized in this report. SAS4A/SASSYS-1 has a growing user base that continues to strengthen the promotion of advanced reactor concepts such as sodium cooled fast reactors. Additional users will help solidify DOE’s leadership role in fast reactor safety both domestically and in international collaborations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Radiation behavior of high-entropy alloys for advanced reactors. Final report

In the first task, we have demonstrated the radiation damage and the recrystallization behaviors in multicomponent alloys through molecular-dynamics simulations. It is found that by alloying with atoms of different sizes, the atomic-level strain increases, and the propensity of the radiation-induced crystalline to amorphous transition increases as the defects cluster in the cascade body. Recrystallization of the radiation induced supercooled or glass regions show that by tuning the composition and the equilibrium temperature, the multicomponent alloys can be healed. The crystalline-amorphous-crystalline transitions predict the potential high radiation resistance in multicomponent alloys. In the second task, three types of high-entropy alloys (HEAs) were fabricated from AlCoCrFeNi and AlCuCrFeNi quinary alloys. Hardness and reduced contact modulus were measured using nanoindentation tests. Heavy ion irradiation were performed using 10 MeV gold and 5 MeV nickel to study radiation effects. Al 0.5 CrCuFeNi 2 shows phase separation upon the presence of copper. Both hardness and contact modulus exhibit the same trend as increasing the applied load, and it indicates that excessive free volume may alter the growth rate of the plastic zone. The as-cast Al 0.1 CoCrFeNi specimen undergone the hot isostatic pressing (HIP) process and steady cooling rate which mitigate the quenching effect. The swelling behavior was characterized by the atomic force microscopy (AFM), and the swelling rate is approximately 0.02% dpa. Selected area diffraction (SAD) patters show irradiation-induced amorphization throughout the ion projected range. Within the peak damage region, an amorpous ring is observed, and a mixture of amorphous/ crystalline structure at deeper depth is found. The Al 0.3 CoCrFeNi HEAs shows good radiation resistance up to 60 peak dpa. No voids or dislocations are observed. The crystal structures remain face-centered-cubic (FCC) before and after 5 MeV Ni irradiation. Higher dpa might be required to study defects formation mechanisms. In the third task, all the constituent binary and ternary systems of the Al-Co-Cr-Fe-Ni system were thermodynamically modeled within the whole composition range. Comparisons between the calculated phase diagrams and literature data are in good agreement. The multi-component thermodynamic database of the Al-Co-Cr-Fe-Ni system was then obtained via extrapolation. The current Al-Co-Cr-Fe-Ni thermodynamic database enables us to carry out the calculations of phase diagrams, which can be used as useful guidelines to identify the Al-Co-Cr-Fe-Ni HEAs with desirable microstructures. In the fourth task, we discuss how as-cast and homogenized phases can be identified, what phases are usually found in the as-cast and homogenized conditions, and what the thermodynamics and kinetics of phase transformations are in the AlCoCrFeNi HEA. The microstructure and phase composition were studied in as-cast and homogenized conditions. It showed the dendritrical structure in the as-cast condition consisting primarily of a nano-lamellar mixture of A2 [disorder body-centered-cubic (BCC)] and B2 (ordered BCC) phases, in addition to a very small amount of A1 [disorder face-centered-cubic (FCC)] phases. The homogenization heat treatment resulted in an increase in the volume fraction of the A1 phase and formation of a Sigma phase. Tensile properties in as-cast and homogenized conditions are reported at 700 °C. Thermodynamic modeling of non-equilibrium and equilibrium phase diagrams for the AlCoCrFeNi HEA gave good agreement with the experimental observations of the phase contents. The reasons for the improvement of ductility after the heat treatment are discussed.

36 MATERIALS SCIENCE↗

Composition Measurements of the HLW HAlG Glasses

This report provides the results from the chemical analyses of the glass compositions of the High-Level Waste High-Aluminum Glass study glasses, a series of simulated nuclear waste glasses designed and fabricated at Pacific Northwest National Laboratory. These data will be used in the development, validation, and implementation of enhanced property/composition models for waste glass vitrification at Hanford. Chemical analyses were performed on a representative sample of each of the quenched glasses to allow for comparisons with targeted compositions. The relative differences between the targeted and measured concentrations of Cr 2 O3, P 2 O 5 , and ZrO 2 for several of the glasses were greater than 10%. The relative difference between the targeted and measured concentrations of CaO was greater than 10% for one glass. The relative difference between the targeted and measured concentrations of Li 2 O was greater than 10% for one glass. These results can be used in further characterization of this series of glasses, including the normalization of Product Consistency Test results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Predicting electrical conductivity in Cu/Nb composites: A combined model-experiment study

The generation of high magnetic fields requires materials with high electric conductivity and good strength properties. Cu/Nb composites are considered to be good candidates for this purpose. In this work, we aim to predict, from theory, the dependence of electric conductivity on the microstructure, most notably on the layer thickness and grain sizes. We also conducted experiments to calibrate and validate our simulations. Bimetal interfaces and grain boundaries are confirmed to have the largest impact on conductivity in this composite material. In this approach, a distribution of the layer thickness is accounted for in order to better model the experimentally observed microstructure. Because layer thicknesses below the mean free path of Cu significantly degrade the conductivity, an average layer thickness larger than expected may be needed to meet conductivity requirements in order to minimize these smaller layers in the distribution. We also investigate the effect of variations in volume fraction of Nb and temperature on the material’s conductivity.

36 MATERIALS SCIENCE↗