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At least 1,405 records · Page 78

Mechanistic Study of the Hydrogen Oxidation/Evolution Reaction over Bimetallic PtRu Catalysts

In this work, the activity of bimetallic PtRu/C with varying amounts of Ru for the hydrogen oxidation/evolution reactions (HOR/HER) was determined. The results demonstrate that surface Ru is not necessary for high activity, which shows that the improved activity of the bimetallic PtRu comes from the electronic interaction of Ru with Pt and the tuning of the hydrogen binding energy (HBE). Using the charge transfer coeffiecient from Butler-Volmer fitting and kinetic modeling, it was determined that Ru affects the HOR/HER mechanism in two ways: changing the pathway from Tafel-Volmer to Heyrovsky-Volmer, and lowering of the activation barrier of the Volmer step. Utilizing catalysts with Heyrovsky-Volmer(RDS) mechanism as well as focusing on tuning the HBE might help improve the activity of non-precious metal catalysts; allowing PGM-free fuel cells to become economically viable.

36 MATERIALS SCIENCE↗

Multi-BGK

This code package solves the multi-species 1D-3V BGK kinetic model of Haack, Hauck, and Murillo [J. Stat. Phys., 168, 2017, Phys. Rev. E, submitted, 2017]. This model conserves mass, momentum, and energy and satisfies Boltzmann's H Theorem, i.e. entropy dissipation. Additionally, the collision model matches either the momentum or temperature relaxation rate of the Boltzmann equation. It can be run in 0D-3V and 1D-3V modes.

Haack, Jeffrey↗

TChem 2.0

The TChem toolkit is an object-oriented C++ software library that enables numerical simulations using complex chemistry and facilitates the analysis of detailed kinetic models. The toolkit provides capabilities for thermodynamic properties and gas-phase and surface chemistry. The computations rely on the Kokkos framework for parallel execution on many-core and GPU-based platforms. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-NA0003525. SAND2021-2752 O

Kim, Kyungjoo↗

TChem-atm v1.0

SAND2024-11300O TChem-atm is a software library that was developed to solve complex kinetic models for atmospheric chemistry applications. TChem-atm interface employs a hierarchical parallelism design to exploit the massive parallelism available from modern computing platforms. It also supports gas atmospheric chemistry applications, e.g., the energy exascale earth system model. TChem can be used as a box model or coupled with a climate model to compute the time evolution of gas tracer species. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525.

Safta, Cosmin↗

Data from Response Surface Methodology Guided Adsorption and Recovery of Free Fatty Acids from Oil Using Resin

The presence of free fatty acids interferes with the conversion of plant oils to biodiesel. Four strong and weak base resins were evaluated for the removal of free fatty acids (FFA) from oil. Amberlite FPA 51 showed the highest adsorption capacity of FFA. A resin concentration above 3% could enable a higher percentage FFA adsorption. The adsorption process fitted a pseudo-first-order kinetic model and achieved equilibrium in approximately 8 h. A full factorial design was used to optimize the resin and FFA concentrations at a fixed temperature (40° C). A ratio of resin to fatty acid concentrations above 1.875 was sufficient for 70% adsorption and the amount adsorbed continued to increase with further added resin. A two-step washing of resin using hexane and ethanol recovered approximately 67.55% ± 4.05% of the initially added fatty acid. The resin that was used was regenerated with 5% NaOH and re-used for a minimum of three consecutive cycles. However, the adsorption capacity diminished to 75% of the initial cycle in cycles 2 and 3. Thus, the work presents a resin-based process for deacidification of oil to reduce fatty acid content of oil for biodiesel production.

Conversion↗

Single-shot picosecond pump coherent Rayleigh scattering thermometry

A single-shot coherent Rayleigh scattering (CRS) technique capable of measurement times less than 10 ns is presented. Here, the use of a mode-locked picosecond pump laser yields repeatable electrostrictive forcing compared to previous CRS experiments using unseeded nanosecond pump pulses, which are beset by shot-to-shot variations. Quantitative measurements are achieved by dispersing the CRS signal onto an EMCCD sensor using a virtually imaged phased array and comparing the experimental spectra to an existing kinetic model with a least-squares fitting routine. Measurements are demonstrated at ambient and low-pressure (2 Torr), low-temperature (100 K) conditions where the CRS measurement is within the collisionless regime. Single-shot statistics indicated precision and accuracy within 4% at ambient conditions and within 8% at low density and temperature conditions. This single-shot CRS technique is a powerful diagnostic tool with potential for multi-parameter measurements in complex flow environments, including high-speed aerodynamic ground test facilities.

Senior, William Charles Bowman [Sandia National La↗

Comparison of two different methods of image analysis for the assessment of microglial activation in patients with multiple sclerosis using (R)-[N-methyl-carbon-11]PK11195

Chronic active multiple sclerosis (MS) lesions have a rim of activated microglia/macrophages (m/M) leading to ongoing tissue damage, and thus represent a potential treatment target. Activation of this innate immune response in MS has been visualized and quantified using PET imaging with [ 11C]-(R)-PK11195 (PK). Accurate identification of m/M activation in chronic MS lesions requires the sensitivity to detect lower levels of activity within a small tissue volume. We assessed the ability of kinetic modeling of PK PET data to detect m/M activity in different central nervous system (CNS) tissue regions of varying sizes and in chronic MS lesions. Ten patients with MS underwent a single brain MRI and two PK PET scans 2 hours apart. Volume of interest (VOI) masks were generated for the white matter (WM), cortical gray matter (CGM), and thalamus (TH). The distribution volume (VT) was calculated with the Logan graphical method (LGM-VT) utilizing an image-derived input function (IDIF). The binding potential (BPND) was calculated with the reference Logan graphical method (RLGM) utilizing a supervised clustering algorithm (SuperPK) to determine the non-specific binding region. Masks of varying volume were created in the CNS to assess the impact of region size on the various metrics among high and low uptake regions. Chronic MS lesions were also evaluated and individual lesion masks were generated. The highest PK uptake occurred the TH and lowest within the WM, as demonstrated by the mean time activity curves. In the TH, both reference and IDIF based methods resulted in estimates that did not significantly depend on VOI size. However, in the WM, the test-retest reliability of BPND was significantly lower in the smallest VOI, compared to the estimates of LGM-VT. These observations were consistent for all chronic MS lesions examined. In this study, we demonstrate that BPND and LGM-VT are both reliable for quantifying m/M activation in regions of high uptake, however with blood input function LGM-VT is preferred to assess longitudinal m/M activation in regions of relatively low uptake, such as chronic MS lesions.

60 APPLIED LIFE SCIENCES↗

Autoencoder Neural Network for chemically reacting systems

Incorporating detailed chemical kinetic models is critical for accurate simulations of reacting flows. However, detailed models involve a large number of thermochemical (TC) state variables. Solving the governing equations to evolve these TC variables becomes impractical for real-world applications. In this work, we propose an autoencoder (AE) neural network (NN)-based reduced model to accelerate such simulations. The AE NN is first trained to find a low-dimensional latent representation of the TC states. Then, the evolving state of a chemical system can be tracked by solving the equations of the latent variables instead of the original TC equations. We demonstrate the reduced model in a syngas CO/H 2 combustion system, using training data collected from canonical perfectly stirred reactors (PSRs). It is found that the AE model can reduce the dimension of the combustion system from 12 to 2 while maintaining low reconstruction error and excellent elemental mass conservation for the test dataset. In the a posteriori test, the combustion states obtained from solving the two latent equations are compared to those from solving the 12 equations of the full model. The AE reduced method is found to be able to capture the diverse combustion states on the top two branches of the S-curve well including the extinction turning point, but with higher prediction errors for states near the ignition turning point.

97 MATHEMATICS AND COMPUTING↗

Using MCNP6 to Estimate Fission Neutron Properties of a Reflected Plutonium Sphere

The purpose of this project was to determine the fission multiplicity distribution, p(v), for the Beryllium Reflected Plutonium (BeRP) ball and to determine whether or not it changed appreciably for various High Density Polyethylene (HDPE) reflected configurations. The motivation for this project was to determine whether or not the average number of neutrons emitted per fission, v, changed significantly enough to reduce the discrepancy between MCNP6 and Robba, Dowdy, Atwater (RDA) point kinetic model estimates of multiplication. The energy spectrum of neutrons that induced fissions in the BeRP ball, NIF (E), was also computed in order to determine the average energy of neutrons inducing fissions, NIF . p(v) was computed using the FMULT card, NIF (E) and NIF were computed using an F4 tally with an FM tally modifier (F4/FM) card, and the multiplication factor, k eff , was computed using the KCODE card. Although NIF (E) changed significantly between bare and HDPE reflected configurations of the BeRP ball, the change in p(v), and thus the change in v, was insignificant. This is likely due to a difference between the way that NIF is computed using the FMULT and F4/FM cards. The F4/FM card indicated that NIF (E) was essentially Watt-fission distributed for a bare configuration and highly thermalized for all HDPE reflected configurations, while the FMULT card returned an average energy between 1 and 2 MeV for all configurations, which would indicate that the spectrum is Watt-fission distributed, regardless of the amount of HDPE reflector. The spectrum computed with the F4/FM cards is more physically meaningful and so the discrepancy between it and the FMULT card result is being investigated. It is hoped that resolving the discrepancy between the FMULT and F4/FM card estimates of NIF(E) will provide better v estimates that will lead to RDA multiplication estimates that are in better agreement with MCNP6 simulations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Simulation of Optical Phenomena in the Upper Atmosphere

This SAND report investigates the electron transport equation in the upper atmosphere and how it relates to auroral light emissions. The electron transport problem is a very stiff boundary value problem, so standard numerical methods such as symmetric collocation and shooting methods will not succeed unless if the boundary conditions are altered with unrealistic assumptions. We show this to be unnecessary and demon- strate a method in which the fast and slow modes of the boundary value problem are essentially decoupled. This allows for an upwind finite difference method to be applied to each mode as is appropriate. This greatly reduces the number of points needed in the mesh, and we demonstrate how this eliminates the need to define new boundary conditions. This method can be verified by showing that under certain restrictive as- sumptions, the electron transport equation has an exact solution that can be written as an integral. The connection between electron transport and the aurora is made explicit and a kinetic model for calculating auroral light emissions is given.

54 ENVIRONMENTAL SCIENCES↗

Aluminum Clad Spent Nuclear Fuel Task 2: Oxide Layer Radiolytic Gas Generation Resolution Experiment Test Plan

This document presents the test plan for Task 2 of the Aluminum Clad Spent Nuclear Fuel Long Term Dry Storage Technical Issues Action Plan. This task’s overarching goal is the resolution of gas generation resulting from the radiolytic degradation of the oxide layers on aluminum. The uncertainty associated with the build-up of gaseous radiolytic products inside the ASNF storage canisters is one of the dominant technical challenges associated with long term dry storage of aluminum clad fuel. The objectives of the Task 2 test plan are to: 1. Understand how radiation chemistry inside the ASNF dry storage canister impacts extended dry storage performance. 2. Understand the radiation induced mechanisms governing the production of radiolytic gases and alteration of gas composition within a canister. 3. Correlate the observed changes in material properties of ASNF with the radiolytic degradation of aluminum oxide in fill environments of variable moisture and gas composition. 4. Compile a predictive kinetic modeling tool, to provide quantitative mechanistic insight into the in-cask radiation chemistry of ASNF. 5. Interface with the canister modeling activity of Task 3 to deliver degradation rates for package performance of both sealed and vented scenarios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Annular Core Research Reactor Pulse History Report: 2003-2017

This report documents and describes the tabulation and analysis of historical pulse operation data from the Annular Core Research Reactor (ACRR) at Sandia National Laboratories (SNL). The pulse data was obtained from a combination of pulse log files generated at the control console and pulse diagnostics system data. The pulses presented were performed within the time period of April 2003 and December 2017. A brief analysis of the data is included to characterize the aggregate behavior of ACRR pulses with respect to theoretical treatments based on the point reactor kinetics model. It is expected that the data presented will provide an organized and consolidated resource to reference historical pulse data at the ACRR for use in analyses, verification and validation, and general understanding of the machine. A comprehensive set of data is presented to the reader in the appendices.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Muons Inc Master CRADA with Annex A for Magnetron Development

Modern CW or pulsed superconducting accelerators of megawatts beams require efficient RF sources controllable in phase and power. It is desirable to have an individual RF power source with power up to hundreds of kW for each Superconductive RF (SRF) cavity. For pulsed accelerators the pulse duration in millisecond range is required. The efficiency of the traditional RF sources (klystrons, IOTs, solid-state amplifiers) in comparison to magnetrons is lower and the cost of unit of RF power is significantly higher. Typically, the cost of RF sources and their operation is a significant part of the total project cost and operation. The magnetron-based RF sources with a cost of power unit of 1-3 dollars per Watt would significantly reduce the capital and operation costs in comparison with the traditional RF sources. This arouses interest in magnetron RF sources for use in modern accelerators. A recently developed kinetic model describing the principle of magnetron operation and subsequent experiments resulted in an innovative technique producing the "stimulated" generation of magnetrons powered below the self-excitation threshold voltage. The magnetron operation in this regime is stable, low noise, controllable in phase and power, and provides higher efficiency than other types of RF power sources. It allows operation in CW and pulse modes (at large duty factor). For pulsed operation this technique does not require pulse modulators to form RF pulses. It also looks as a promising opportunity to extend magnetron life time.

43 PARTICLE ACCELERATORS↗

Report on the FY20 Characterization of Age Hardened Alloy 709 Materials

This report provides the results on microstructural characterization of the first commercial heat of Alloy 709 plate material undergone additional age hardening treatment. In FY19, through thermodynamic-kinetic modeling and microstructural characterization, it is determined that the 775°C/10 h age-hardening treatment can promote desired precipitation on dislocations and has the potential to further improve the mechanical performance of the material. In FY20, the treatment protocol was applied to the ESR-1150°C condition, and the microstructure was then compared with the ESR-1100°C condition. It was found that the 1150°C solution annealing (SA) dramatically reduced the dislocation density compared to the 1100°C SA, resulting a smaller number density of Nb-rich fine precipitates which grow on dislocations during the age hardening treatment. Other features are very similar between the two. The effect of age hardening on creep performance is discussed. In addition, TEM characterization of a creep-ruptured sample (600°C/330 MPa) was performed. Specimens from the grip region and the gauge region was studied. The grip region specimen was effectively aged at 600°C for extended period, while the gauge region specimen was mechanically deformed at 600°C. The microstructures are very different, implying the importance of a dynamical effect on precipitation.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Pulse Detonation Engine for Advanced Oxy-Combustion of Coal-Based Fuel for Direct Power Extraction Applications

Pressure gain combustion and magnetohydrodynamic (MHD) systems have the potential to provide a step increase in the efficiency of combined-cycle power plants. Specific advantages include a net pressure increase to the system instead of a pressure drop, the high temperature of the detonation waves can increase the efficiency of power extraction compared to other processes, significant thermal energy can be released in a compact region, and the high velocities of the flow increase extraction of electrical power. In summary, a pressure gain combustor coupled with a MHD has the potential to be transformative. Despite the potential advantages, relatively little research has been conducted considering coupled pressure gain combustion systems with MHD systems. With this background and motivation, the overall goal of this effort was to advance the knowledge, technology, and computational tools associated with coupled detonation and MHD systems. A joint experimental and computational approach was used while seeking to accomplish the goals of this work. Specifically, two pulse detonation engines were developed and used for the experiments to produce detonations. Detonation speeds were measured for a variety of flow and fuel conditions (e.g., methane, propane, with coal particles). Preliminary electrical conductivity measurements were collected. An extensive amount of research was performed to identify sensitivities of detonation behaviors to the presence of combustion products. Computationally, a twofold approach was used in this work. First, a solver was developed for solving the governing equations for a reactive flow with coupled detonation and ionization chemistry. The solver was applied to study the impacts of seed material ionization on detonation. Second, a conservation element-solution element (CE-SE) based numerical solver for detonation studies with a reduced reaction mechanism for oxy-methane combustion was developed and verified on standard test cases. Key findings and contributions from this work are as follows. A system was developed for injecting powderized coal, or other seeding material, into a pulse-detonation system. The influence of a combustion product (i.e., CO 2 ) on detonation behavior was identified. Knowledge gained from this work is applicable to devices such as rotating detonation engines, where combustion products mix with fresh reactants. A system for measuring the electrical conductivity of the exhaust from a pulse-detonation engine was developed. The open-source solver, Clawpack, was extended to solve the reactive Euler equations for simulating detonations. A coupled combustion and ionization chemistry was developed in a single chemical kinetic model for methane oxidation. This model can be used to solve coupled MHD and detonation simulations. It was found that parasitic interactions from ionization chemistry with the magnetic field can reduce the detonation velocity by up to 8%, with a potential impact on power extraction of 15%. It is recommended that interactions between the detonation front and MHD field be considered. Higher gas temperatures and velocities were achieved owing to oxy-fuel detonations. Use of radical dissociation reactions in the reduced reaction mechanism, was found to be critical in predicting detonation temperature and velocity accurately.

01 COAL, LIGNITE, AND PEAT↗

Increasing melt efficiency and secondary alloy usage in aluminum die casting

In this project, the focus was to develop thermodynamic and kinetic models for the aluminum melting process involving secondary alloys, refractory materials and flux materials. The major research outcome of this study is 1) the refractory composition of CaO (8-12%), microsilica (1-3%), BaSO 4 and/or BaO (no more than 5%), B 2 O 3 (5%) and Al 2 O 3 (balance) effectively reduced the reactions with liquid Al and alloying/impurity elements and heat transfer during melting and holding process. 2) a flux composition of NaCl-KCl-(1-10%)KAlF 4 exhibited an effective covering effect and prevented the dross formation during melting of Al process. 3) A high Fe (0.44%) content recycled Al alloy with compatible mechanical properties was developed based on the impurities control methods, which provides great potential to replace the commercial structural alloys from primary Al and increase the usage of secondary alloys.

36 MATERIALS SCIENCE↗

Evaluation of AddUp Precision L-PBF Technology for Tooling and Other Industrial Applications

ORNL (Contractor) and AddUp Inc. (Participant) collaborated to enable the adoption of laser powder bed fusion for tooling applications, critical for reshoring the manufacturing sector in the U.S. Most of the work on laser powder bed fusion has focused on high value materials such as Ti-6Al-4V and Inconel 718 for niche applications in aerospace, biomedical and energy sectors. In this collaboration, ORNL and AddUp worked laser powder bed fusion of maraging steels for tooling applications while leveraging the unique ability of the AddUp laser powder bed fusion system to deposit fine powders. We demonstrated that the AddUp technology is capable of depositing complex artifacts and features such as overhangs within desired tolerances. We also showed that direct aging of the deposited parts result in simultaneously higher strength and elongation compared to the conventional two step heat treatments, which could result in significant energy savings. Finally, we developed thermos-kinetic models to enable design of heat treatments for optimal material properties compared to the energy intensive empirical methods currently used. The report summarizes the detailed findings of this collaboration.

36 MATERIALS SCIENCE↗

Gas-phase Radiolysis in Plutonium Dioxide Powder

A sample of PuO 2 powder undergoes self radiolysis, causing water present in the solid to generate hydrogen, oxygen, and minor species (e.g. H 2 O 2 ). This is a matter of concern for stored PuO 2 , since the gases could react exothermically and rupture the container. In experiments at LANL, most PuO 2 /salt samples generate mostly H 2 , but a few samples generate a mixture of H 2 and O 2 together. In these special cases, the mixture of H 2 and O 2 in the pore volumes of the powder will then be subject to radiolysis, causing the reverse reaction H 2 + O 2 $\Rightarrow$ H 2 O. In order to understand the steady-state quantities of these gases, it is necessary to estimate the amount of energy from the alpha irradiation that drives this reaction. This report outlines one possible approach for this process, yielding a value for the fractional amount of radiation deposited in the gas phase of 294 ppm. This corresponds to the case of a powder with porosity of 78%. We then use a comprehensive chemical kinetics model based on elementary gas phase reactions to calculate the rate of conversion back to water. We estimate a reduction in the H 2 pressure of about 12 kPa/month, which applies only when O 2 is simultaneously present in the gas phase.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗