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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Interference between Franck–Condon and Herzberg–Teller Terms in the Condensed-Phase Molecular Spectra of Metal-Based Tetrapyrrole Derivatives

The commonly used Franck-Condon (FC) approximation is inadequate for explaining the electronic spectra of compounds that possess vibrations with substantial Herzberg-Teller (HT) couplings. Metal-based tetrapyrrole derivatives, which are ubiquitous natural pigments, often exhibit prominent HT activity. In this paper, we compare the condensed phase spectra of zinc-tetraphenylporphyrin (ZnTPP) and zinc-phthalocyanine (ZnPc), which exhibit vastly different spectral features in spite of sharing a common tetrapyrrole backbone. The absorption and emission spectra of ZnTPP are characterized by a lack of mirror symmetry and nontrivial temperature dependence. In contrast, mirror symmetry is restored, and the nontrivial temperature-dependent features disappear in ZnPc. We attribute these differences to FC-HT interference, which is less pronounced in ZnPc because of a larger FC component in the dipole moment that leads to FC-dominated transitions. A single minimalistic FC-HT vibronic model reproduces all the experimental spectral features of these molecules. These observations suggest that FC-HT interference is highly susceptible to chemical modification.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Critical Experiment Design Phase 2 Report for Integral Request 304

This report documents the second phase of the critical experiment design process (CED-2) conducted as part of integral experiment request (IER) 304. The purpose of IER-304 is to develop a temperature-dependent critical experiment capability at the Sandia National Laboratories critical experiment facility using low-enriched uranium oxide fuel. Only a few benchmark quality critical experiments are currently available to validate criticality safety computational methods at temperatures other than room temperature. Recent advancements in computational techniques such as implementation of on-the-fly Doppler broadening techniques and advanced treatment of thermal scattering data necessitate the development of additional experimental capabilities in this area. The work described in this report developed representative configurations using 7uPCX and BUCCX fuels, analyzed the physics exercised by the different arrays, and analyzed the estimated experimental uncertainties. This report also scopes the information necessary for performing modifications to the reactor to accommodate operation at elevated and reduced temperatures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Quantifying model prediction sensitivity to model-form uncertainty

Computational and mathematical models are essential to understanding complex systems and phenomena. However, when developing such models, limited knowledge and/or resources necessitates the use of simplifying assumptions. It is therefore crucial to quantify the impact of such simplifying assumptions on the reliability and accuracy of resulting model predictions. This work develops a first-of-its-kind approach to quantify the impact of physics modeling assumptions on predictions. Here, we leverage the emerging field of model-form uncertainty (MFU) representations, which are parameterized modifications to modeling assumptions, in combination with grouped Sobol’ indices to quantitatively measure an assumption’s importance. Specifically, we compute the grouped Sobol’ index for the MFU representation’s parameters as a single importance measure of the assumption for which the MFU representation characterizes uncertainty. To ensure this approach is robust to the subjective choice of how to parameterize a MFU representation, we establish bounds for the difference between sensitivity results for two different MFU representations based on differences in model prediction statistics. The capabilities associated with this approach are demonstrated on three exemplar problems: an upscaled subsurface contaminant transport problem, ablation modeling for hypersonic flight, and nuclear waste repository modeling. We found that our grouped approach is able to assess the impact of modeling assumptions on predictions and offers computational advantages over classical Sobol’ index computation while providing more interpretable results.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Heat Exchanger Design for Waste Heat Recovery using Additive Manufacturing

With anticipated increases in global energy use and their associated emissions, there are many efforts to improve the emissions and efficiency of many industrial processes through waste heat recovery (WHR). To maximize improvements, the heat exchangers in WHR power cycles must be designed and optimized for a given heat source. Meanwhile, additive manufacturing (AM) is a single part manufacturing technique that provides the opportunity to develop unique and complex heat exchanger designs. Consequently, this work centers on the modeling, design, optimization, and testing of AM shell and tube heat exchangers for WHR. Specifically, a modified one-dimensional (1+1-D) and three-dimensional (3-D) heat exchanger models were developed and validated, with the 1+1-D model serving as the basis for design optimization. After modifications to the design to allow for AM, heat exchanger geometry optimizations were completed, targeting increased effectiveness across a range of physical parameters. Of the designs considered, nine were additively manufactured using Ti5553, and then tested using an external heat source and working fluid. Experimentally, the nineteen-tube, zero-baffle heat exchanger displayed the best overall performance, with the effects of dimensional accuracy, surface roughness, and baffles in the other designs also indicated. Next, the experimental results were used as inputs for the 1+1-D model. Although the original model was able to predict fluid outlet temperatures within 5% differences, larger variations in the heat exchanger performance parameters, temperature differences, and pressure drop necessitated optimizing the pressure drop and heat transfer calculations within the model. Thus, the resulting improved model was able to predict the heat transfer rates, heat source temperature difference, and effectiveness within 15% differences, while showing improvements in the pressure drops and working fluid temperature differences. The improved model serves as the foundation for future work to improve the design and performance of AM heat exchangers.

Spickler, Bailey Ann↗
DOE OSTI2026

Impact of new physics on the JUNO-long-baseline synergy in the neutrino mass ordering determination

The determination of the neutrino mass ordering is one of the flagship goals in particle physics. A well-known and powerful synergy emerges when combining high-precision measurements of the effective atmospheric mass-squared splitting from electron antineutrino disappearance in reactor experiments with that from muon (anti)neutrino disappearance in accelerator-based long-baseline experiments. To fully exploit this synergy, percent-level precision in the atmospheric mass splitting is required—a target that JUNO is expected to achieve within a few months of data taking. This motivated the formulation of a mass ordering sum rule for neutrino disappearance channels, which shows that by combining data from T2K and NOvA with JUNO after one year of operation, the neutrino mass ordering can be determined at the 3⁢𝜎 confidence level. Since JUNO has recently started taking data, it is timely to ask whether this sum rule remains robust in the presence of new physics. We identify the necessary conditions for new physics to affect the sum rule and demonstrate that, in some cases, such effects could lead to an incorrect inference of the mass ordering. As concrete examples, we consider scalar nonstandard interactions (SNSI) and neutrinos coupled to an ultralight scalar field. We find that, for SNSI, current constraints render any modification of the sum rule negligible, whereas in the latter case, the inference of the ordering requires caution. Nevertheless, these effects can be disentangled, illustrating how the sum rule can also be used to search for new physics.

Alves, Gustavo F. S. [Fermi National Accelerator L↗
DOE OSTI2023

Comprehensive Review of DPF-based Flash Neutron Radiography Viability

MJOLNIR (MegaJOule Neutron Imaging Radiography) is a Dense Plasma Focus (DPF) being developed by LLNL as a prototype to assess the viability of a DPF as a flash neutron radiography source. To date, MJOLNIR has discharged up to 1.3 MJ of stored energy into a deuterium plasma load and achieved yields up to 1.2 × 10 12 neutrons per discharge. The MJOLNIR pulse length already meets the preliminary requirements for flash neutron radiography and we demonstrate in this report plausible paths forward to meet the yield requirement in a deuterium plasma. MJOLNIR’s neutron spot size has been characterized to be a factor of two greater than radiography requirements and presents the greatest challenge. A path forward to sufficiently shrinking spot size is outlined in this report, using a combination of gas dopants and a smaller anode implosion radius. A DPF is a plasma device with coaxial electrodes whose discharge ends with a stagnated hot and dense plasma column on-axis, at the tip of the central anode. Inside the MJOLNIR DPF plasma column, both thermal and beam target processes generate neutrons. To understand the underlying physics of neutron generation inside the DPF, we model the experiment using a combination of kinetic, fluid, and reduced-order models we have been developing for over ten years at LLNL. Our numerical tools are also pivotal to charting the path forward because they allow us to numerically test out which modifications would improve the DPF’s characteristic output.

42 ENGINEERING↗
DOE OSTI2022

Simultaneously Enhanced Hydrophilicity and Stability of a Metal-Organic Framework via Post-Synthetic Modification for Water Vapor Sorption/Desorption

With increasing demands for high-performance water sorption materials, metal-organic frameworks (MOFs) have gained considerable attention due to their high maximum uptake capacities. In many cases, however, high overall capacity is not necessarily accomplishing high working capacity under operating conditions, due to insufficient hydrophilicity and/or water stability. Herein, we present a post-synthetic modification (PSM) of MOF-808, with di-sulfonic acids enhancing simultaneously its hydrophilicity and water stability without sacrificing its uptake capacity of ≈30 mmol g -1 . Further, di-sulfonic acid PSM enabled a shift of the relative humidity (RH) associated with a sharp step in water vapor sorption from 35–40 % RH in MOF-808 to below 25 % RH. While MOF-808 lost uptake capacity and crystallinity over multiple sorption/desorption cycles, the di-sulfonic acid PSM MOF-808 retained >80 % of the original capacity. PSM MOF-808 exhibited good hydrothermal stability up to 60 °C and high swing capacity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

The anomaly that was not meant IIB

Type IIB supergravity enjoys a discrete non-Abelian duality group, which has potential quantum anomalies. In this paper we explicitly compute these, and present the bordism group that controls them, modulo some physically motivated assumptions. Quite surprisingly, we find that they do not vanish, which naively would signal an inconsistency of F-theory. Remarkably, a subtle modification of the standard 10d Chern-Simons term cancels these anomalies, a fact which relies on the specific field content of type IIB supergravity. We also discover other ways to cancel this anomaly, via a topological analog of the Green-Schwarz mechanism. These alternative type IIB theories have the same low energy supergravity limit as ordinary type IIB, but a different spectrum of extended objects. They could either be part of the Swampland, or connect to the standard theory via domain walls.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2026

Impact of New Physics on the JUNO-Long-Baseline Synergy in Neutrino Mass Ordering Determination

The determination of the neutrino mass ordering is one of the flagship goals in particle physics. A well-known and powerful synergy emerges when combining high-precision measurements of the effective atmospheric mass-squared splitting from electron antineutrino disappearance in reactor experiments with that from muon (anti)neutrino disappearance in accelerator-based long-baseline experiments. To fully exploit this synergy, percent-level precision in the atmospheric mass splitting is required-a target that JUNO is expected to achieve within a few months of data taking. This motivated the formulation of a mass ordering sum rule for neutrino disappearance channels, which shows that by combining data from T2K and NOvA with JUNO after one year of operation, the neutrino mass ordering can be determined at the $3σ$ confidence level. Since JUNO has recently started taking data, it is timely to ask whether this sum rule remains robust in the presence of new physics. We identify the necessary conditions for new physics to affect the sum rule and demonstrate that, in some cases, such effects could lead to an incorrect inference of the mass ordering. As concrete examples, we consider Scalar Non-Standard Interactions (SNSI) and neutrinos coupled to an ultralight scalar field. We find that, for SNSI, current constraints render any modification of the sum rule negligible, whereas in the latter case, the inference of the ordering requires caution. Nevertheless, these effects can be disentangled, illustrating how the sum rule can also be used to search for new physics.

Alves, Gustavo F.S. [Fermilab; Northwestern U.; Sa↗
DOE OSTI2021

Design Status Update of the Electron-Ion Collider

The design of the electron-ion collider EIC to be constructed at Brookhaven National Laboratory has been continuously evolving towards a realistic and robust design that meets all the requirements set forth by the nuclear physics community in the White Paper. Over the past year activities have been focused on maturing the design, and on developing alternatives to mitigate risk. These include improvements of the interaction region design as well as modifications of the hadron ring vacuum system to accommodate the high average and peak beam currents. Beam dynamics studies have been performed to determine and optimize the dynamic aperture in the two collider rings and the beam-beam performance. We will present the EIC design with a focus on recent developments.

43 PARTICLE ACCELERATORS↗
DOE OSTI2020

The Influence of Ozone: Superstoichiometric Oxygen in Atomic Layer Deposition of Fe 2 O 3 Using tert -Butylferrocene and O 3

Understanding the chemical mechanisms at play in atomic layer deposition (ALD) is critical for effective process development and expansion of ALD into more complex classes of materials. In this work, a mechanistic study of iron oxide deposited by ALD using tert-butylferrocene and ozone as reactants is performed. Iron oxide ALD using ozone is a useful model system for mechanistic studies due to the prevalence of ozone-based ALD processes and the uses of iron oxide in ternary and quaternary metal oxides. Results show that saturation conditions require significantly greater exposures of both reactants than is typically reported in the literature, and growths per cycle of greater than one monolayer of Fe 2 O 3 per cycle are observed and explained. A growth mechanism is proposed whereby increased ozone exposure results in uptake of superstoichiometric oxygen into the film. X-ray characterizations reveal the presence of excess oxygen stored near the surface of films deposited with larger ozone exposures and show that increased ozone exposures cause crystalline domain rearrangement and conversion of the film from the γ-maghemite phase to the α-hematite phase. The mechanism described here has implications for the wider class of ozone-based ALD processes, and potential applications of this growth phenomenon are discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Catalytic Consequences of Hierarchical Pore Architectures within MFI and FAU Zeolites for Polyethylene Conversion

The benefits of hierarchical zeolites for the conversion of bulky molecules like polymeric waste have been reported in the literature; however, the impact of mesopore sizes and connectivities on rates, product selectivities, and catalyst deactivation in the context of plastic upcycling has not been systematically probed. Here, in this study, we synthesized a suite of hierarchical MFI and FAU zeolites via desilication under varying conditions for metal-free polyethylene conversion reactions under batch and flow conditions (473–523 K). Polyethylene (solid) conversion rates (normalized by Bro̷nsted acid site density) were higher on hierarchical than parent microporous MFI regardless of mesopore connectivities, i.e., open or constricted, suggesting that the incorporation of mesopores facilitates diffusion of intermediate products to access medium-pore protons for successive scission events. Furthermore, higher branched:linear gaseous product ratios were produced on hierarchical than parent MFI, since mesopores allow for egress of bulkier molecules without undergoing further secondary events, e.g., isomerization back to linear alkanes/alkenes or beta scission. Solid conversion rates on hierarchical FAU synthesized via desilication with cetyltrimethylammonium bromide (CTABr), however, were not higher than parent FAU, likely because the presence of CTABr facilitates recrystallization of leached species to form composites (hierarchical FAU and ordered mesoporous materials) with more isolated mesopores. The stagnation in rates, despite increased mesopore volumes (>0.22 cm 3 g –1 ), highlights the importance of confinement effects provided by micropores for cleaving C–C bonds at modest reaction conditions. In situ 1 H MAS NMR performed on polyethylene with MFI zeolite show that PE isomerizes (and potentially deconstructs) at temperatures near 450 K, highlighting the role of Bro̷nsted acid sites in activating C–C bonds under mild reaction conditions. Catalyst recyclability studies showed that all catalysts undergo deactivation during plastic upcycling reactions, but to varying extents. Overall, hierarchical materials have better catalyst stability than parent materials, although the differences in stability between hierarchical and parent FAU are smaller than those for MFI. Taken together, these findings demonstrate how rates, selectivities, and catalyst deactivation from plastic upcycling reactions can be controlled via fine-tuning the identity and connectivity of mesopores.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Novel method to control explosive shock sensitivity: Formulations, experiments and modeling

The microstructure of a heterogeneous high explosive (HE) affects its shock initiation sensitivity and detonation performance. Alteration of the void content and/or void structure (i.e., bulk heating or mechanical damage) therefore changes the shock initiation behavior. Controlling and predicting the change in shock sensitivity after an HE has undergone microstructural changes addresses an important and challenging goal for the design and understanding of novel energetic material formulations. In this study, we aimed to develop HE systems to precisely tune shock sensitivity by a thermal treatment prior to use. Specifically, we incorporated a small fraction (1 wt% or less) of thermally expandable microspheres (TEMs) during the formulation process of various plastic-bonded explosives (PBX). TEMs typically consist of a thermoplastic acrylonitrile shell (10-50 µm diameter), which encapsulates an inert low boiling hydrocarbon. Upon heating, the TEMs expand as the shell softens while the hydrocarbon gasifies, increasing the internal pressure and expanding the particle by as much as 120 vol% (irreversibly). Here, we present our progress on shock sensitivity comparisons of HE formulations doped with TEMs after heating and expansion. Experiments, using Composition C-4 thermally cycled to 120°C, showed an increase in shock sensitivity. Additionally, mesoscale modeling revealed that the TEM itself does not act as a hotspot, but instead has a secondary effect on the response of nearby voids. We conclude that TEMs indeed do provide a method to tune shock sensitivity. Further, our results emphasize the non-uniformity of shock waves at the mesoscale, and that upstream defects influence the reactivity of downstream defects.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Evaluation of High Level Waste Sludge Processing Behavior

The U.S. Department of Energy’s (DOE) Hanford Site has 177 underground storage tanks that contain wastes from past nuclear fuel reprocessing and waste-management operations. Over 20% of this waste is in the form of an insoluble sludge that will require slurry modification before its transfer to the Waste Treatment and Immobilization Plant (WTP). Specific WTP acceptance criteria for waste feed delivery describe the physical and chemical characteristics of the waste that must be met before the waste is transferred to the WTP. One challenging requirement relates to the undissolved solids (UDS) composition in a waste feed because the waste contains solid particles that settle, and their concentration and relative proportion can change during the transfer of the waste in individual batches. A key uncertainty is the ability to transfer and mix wastes with large variations in UDS concentrations and resulting settling rates. To address this uncertainty, a number of small scale mixing and settling tests have been conducted to determine the mobilization performance of variable chemistry simulants. Comparison of the size and density of the particulate for each simulant to that of southeast area Hanford sludge was made using metrics for particle mobilization, suspension, settling, and pipeline transfer where dependance on particle size and density may be different, including: 1. Settling velocity, 2. Critical shear stress for erosion, 3. Just-suspended impeller speed, and 4. Pipeline critical transport velocity. Existing high-level waste sludge data has shown the effect that increasing Al concentration has on resulting settled solids. This differential settling of particles in the sludge has the possibility of resulting in solids segregation during feed preparation and uneven particle distribution during pipeline transportation or mixer jet pump operations. Understanding the predictive capabilities of HLW solids settling and transport as well as potential remedies for addressing disparate sludge behaviors can help provide technical guidance during HLW flowsheet planning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2020

Boosting alkaline hydrogen evolution: the dominating role of interior modification in surface electrocatalysis

The alkaline hydrogen evolution reaction (A-HER) holds great promise for clean hydrogen fuel generation but its practical utilization is severely hindered by the sluggish kinetics for water dissociation in alkaline solutions. Traditional ways to improve the electrochemical kinetics for A-HER catalysts have been focusing on surface modification, which still can not meet the demanding requirements for practical water electrolysis because of catalyst surface deactivation. In this work, we report an interior modification strategy to significantly boost the A-HER performance. Specifically, a trace amount of Pt was doped in the interior Co 2 P (Pt–Co 2 P) to introduce a stronger dopant–host interaction than that of the surface-modified catalyst. Consequently, the local chemical state and electronic structure of the catalysts were adjusted to improve the electron mobility and reduce the energy barriers for hydrogen adsorption and H–H bond formation. As a proof-of-concept, the interior-modified Pt–Co 2 P shows a reduced onset potential at near-zero volts for the A-HER, low overpotentials of 2 mV and 58 mV to achieve 10 and 100 mA cm –2 , and excellent durability for long-term utilization. The interior-modified Pt–Co 2 P delivers superior A-HER performance to Pt/C and other state-of-the-art electrocatalysts. This work will open a new avenue for A-HER catalyst design.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Particle resonances in toroidal fusion devices

Resonances of high energy particles in magnetic confinement devices due to electromagnetic instabilities can strongly modify the distribution, leading to a reduction in fusion power and even discharge termination and particle loss to the device walls through avalanche. The existence of a mode particle resonance depends on properties of the equilibrium, particle trajectories, and perturbation mode harmonic content. Resonance location is a function of particle energy and equilibrium field line helicity. Different methods for finding resonance location and energy dependence are developed. The properties of resonances are discussed using examples from magnetic fusion devices. Here, we show that if mode resonances exist at low particle energy, they very likely also exist at high energy, thus modifying high energy beam particles and fusion products. It is possible for a resonance to appear due to mode induced orbit helicity modification when it is forbidden at low mode amplitude.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗