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DOE OSTI2021

Construction of Lattice Strain in Bimetallic Nanostructures and Its Effectiveness in Electrochemical Applications

Bimetallic nanocrystals (NCs), associated with various surface functions such as ligand effect, ensemble effect, and strain effect, exhibit superior electrocatalytic properties. The stress-induced surface strain effect can alter binding strength between the surface active sites and reactants as well as their intermediates, and the electrochemical performance of bimetallic NCs can be significantly facilitated by the lattice-strain modification via their morphologies, sizes, shell-thickness, surface defectiveness as well as compositions. Here in this review, an overview of fundamental principles, characterization techniques, and quantitative determination of the surface lattice strain is provided. Various strategies and synthesis efforts on creating lattice-strain-engineered bimetallic NCs, including the de-alloying process, atomic layer-by-layer deposition, thermal treatment evolution, one-pot synthesis, and other efforts are also discussed. It is further outlined how the lattice strain effect promotes electrochemical catalysis through the selected case studies. The reactions on oxygen reduction reaction, small molecular oxidation, water splitting reaction, and electrochemical carbon dioxide reduction reactions are focused. In particular, studies of lattice strain arisen from core–shell nanostructure and defectiveness are highlighted. Lastly, the potential challenges are summarized and the prospects of lattice-strain-based engineering on bimetallic nanocatalysts with suggestion and guidance of the future electrocatalyst design are envisioned.

36 MATERIALS SCIENCE↗

NASA NTRS1977

Evolution of the moon: The 1974 model

The interpretive evolution of the moon can be divided now into seven major stages beginning sometime near the end of the formation of the solar system. These stages and their approximate durations in time are as follows: (1) The Beginning: 4.6 billion years ago, (2) The Melted Shell: 4.6 to 4.4 billion years ago, (3) The Cratered Highlands: 4.4 to 4.1 billion years ago, (4) The Large Basins: 4.1 to 3.9 billion years ago, (5) The Light-colored Plains: 3.9 to 3.8 billion years ago, (6) The Basaltic Maria: 3.8 to 3.0(?) billion years ago, and (7) The Quiet Crust: 3.0(?) billion years ago to the present. The contributions of the Apollo and Luna exploration toward the study of those stages of evolution are reviewed.

Schmitt, H. H.↗

DOE OSTI2025

Impact of the Latest 22 Ne+ α Reaction Rates on Nucleosynthesis in Massive Stars and Galactic Chemical Evolution

In massive stars (initial mass of ≳9 M ⊙ ), the weak s- (slow neutron capture) process produces elements between Fe and Zr, enriching the Galaxy with these elements through core-collapse supernova explosions. The weak s-process nucleosynthesis is driven by neutrons produced in the 22 Ne(α, n) 25 Mg reaction during convective He core and C shell burning. The yields of heavy elements thus depend on the 22 Ne(α, n) 25 Mg and the competitive 22 Ne(α, γ) 26 Mg reaction rates, which are dominated by several narrow-resonance reactions. While the accuracy of these rates has been under debate for decades, recent experimental efforts, including ours, drastically reduced these uncertainties. In this work, we use a set of 280 massive star nucleosynthesis models calculated using different 22 Ne(α, n) 25 Mg and 22 Ne(α, γ) 26 Mg rates and a galactic chemical evolution (GCE) study to probe their impact on the weak s-process elemental abundances in the Galaxy. The GCE was computed with the OMEGA+ code, using the new sets of stellar yields with different 22 Ne+α rates. From GCE, we find that these rates are causing up to 0.45 dex of variations in the [Cu/Fe], [Ga/Fe], and [Ge/Fe] ratios predicted at solar metallicity. The greatest impact on the stellar nucleosynthesis and GCE results derives from uncertainties in the (α, n) strength (ωγ (α,n) ) of the E x = 11.32 MeV resonance. We show that variations observed in the GCE calculations for weak s-process elements become negligibly smaller than dispersions found in observations once the ωγ (α,n) is accurately determined within the uncertainty of 10%–20% (typically reported experimental errors for the resonance) in future nuclear physics experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

First spectroscopic study of odd-odd Cu 78

Nuclei in the vicinity of 78 Ni are important benchmarks for nuclear structure, which can reveal changes in the shell structure far from stability. Spectroscopy of the odd-odd isotope 78 CU was performed for the first time in an experiment with the EURICA setup at the Radioactive Isotope Beam Factory at RIKEN Nishina Center. Excited states in the neutron-rich isotope were populated following the β decay of 78 Ni produced by in-flight fission and separated by the BigRIPS separator. A level scheme based on the analysis of $\gamma$-$\gamma$ coincidences is presented. Tentative spin and parity assignments were made when possible based on the β -decay feeding intensities and $\gamma$-decay properties of the excited states. Time correlations between β and $\gamma$ decay show clear indications of an isomeric state with a half-life of 3.8(4) ms. Large-scale Monte Carlo shell-model calculations were performed using the A3DA-m interaction and a valence space comprising the full f p shell and the 1⁢g 9/2 and 2⁢d 5/2 orbitals for both protons and neutrons. The comparison of the experimental results with the shell-model calculations allows interpreting the excited states in terms of spin multiplets arising from the proton-neutron interaction. In conclusion, the results provide further insight into the evolution of the proton single-particle orbitals as a function of neutron number, and quantitative information about the proton-neutron interaction outside the doubly magic 78 Ni core.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS1985

Molecular cloud evolution and star formation

The present state of knowledge of the relationship between molecular clouds and young stars is reviewed. The determination of physical parameters from molecular line observations is summarized, and evidence for fragmentation of molecular clouds is discussed. Hierarchical fragmentation is reviewed, minimum fragment scales are derived, and the stability against fragmentation of both spherically and anisotropically collapsing clouds is discussed. Observational evidence for high-velocity flows in clouds is summarized, and the effects of winds from pre-main sequence stars on molecular gas are discussed. The triggering of cloud collapse by enhanced pressure is addressed, as is the formation of dense shells by spherical outflows and their subsequent breakup. A model for low-mass star formation is presented, and constraints on star formation from the initial mass function are examined. The properties of giant molecular clouds and massive star formation are described. The implications of magnetic fields for cloud evolution and star formation are addressed.

Silk, J.↗

NASA NTRS1994

Search for important weak interaction nuclei in presupernova evolution

A search is made for the most important electron captures and beta-decays after core silicon burning in massive stars. A nuclear statistical equilibrium code is used to compute isotopic abundances. Electron capture and beta-decay rates are estimated for the 150 most abundant isotopes in a simplified fashion which generally includes the strongest transitions. These estimates are made for nuclei in the fp-shell and use techniques similar to Fuller, Fowler, & Newman (1982a), and are compared to them. The general behavior of the rate of change of Y(sub e) is examined. These methods are then used to follow a typical stellar trajectory, seeking the most important weak interactions during the formation of the iron core. Ranked lists of nuclei are given, to prioritize more detailed studies on individual nuclei. Beta-decays are found to ben an important modification to the evolution below the rate of change of Y(sub e) approx. = 0.46 as the core approaches a state of dynamic equilibrium between electron captures and beta-decays.

Aufderheide, Maurice B.↗

NASA NTRS1994

Self-gravity and dissipation in polar rings

Studies of inclined rings inside galaxy potentials have mostly considered the influence of self-gravity and viscous dissipation separately. In this study, we construct models of highly inclined ('polar') rings in an external potential including both self-gravity and dissipation due to a drag force. We do not include pressure forces and thus ignore shock heating that dominates the evolution of gaseous rings inside strongly nonspherical potentials. We adopt an oblate spheroidal scale-free logarithmic potential with axis ratio q = 0.85 and an initial inclination of 80 deg for the self-gravitating rings. We find that stellar (dissipationless) rings suffer from mass loss during their evolution. Mass loss also drives a secular change of the mean inclination toward the poles of the potential. As much as half of the ring mass escapes in the process and forms an inner and an outer shell of precessing orbits. If the remaining mass is more than approximately 0.02 of the enclosed galaxy mass, rings remain bound and do not fall apart from differential precession. The rings precess at a constant rate for more than a precession period tau(sub p) finding the configuration predicted by Sparke in 1986 which warps at larger radii toward the poles of the potential. We model shear viscosity with a velocity-dependent drag force and find that nuclear inflow dominates over self-gravity if the characteristic viscous inflow time scale tau(sub vi) is shorter than approximately 25(tau(sub p)). Rings with (tau(sub vi))/(tau(sub p)) less than or approximately equal to 25 collapse toward the nucleus of the potential within one precession period independent of the amount of self-gravity. Our results imply that stars and gas in real polar rings exhibit markedly different dynamical evolutions.

Dubinski, John↗

DOE OSTI2025

Control of core–shell nanoparticles properties through plasma synthesis: a computational study

The improved properties of core–shell nanoparticles (CSNPs) over homogeneous nanoparticles (NPs) have expanded and diversified the applications of these nanomaterials. However, controlling the properties of CSNPs can be a challenging task. Low temperature plasmas have proven to be an effective method of producing NPs with uniform size and morphology, and high yield. That said, NP transport and growth dynamics are sensitive to LTP properties. We report on a computational investigation of the evolution of Ge–Si CSNP properties as a function of operating conditions through the modeling of a flowing, two-zone inductively coupled plasma (ICP) reactor. Ar/GeH 4 and Ar/SiH 4 gas mixtures were supplied to separate plasma zones at a pressure of 1 Torr to promote growth of Ge cores and Si shells. The negatively charged CSNPs are trapped electrostatically in the vicinity of the antennas where the plasma is generated and where the majority of particle growth occurs. Particles that grow to a critical size are then de-trapped by fluid drag due to neutral gas flow. A two-dimensional hybrid plasma model coupled with a three-dimensional kinetic NP transport model were utilized to resolve plasma chemistry and NP growth processes that take place on distinct timescales. The trends in CSNP properties and trapping mechanisms associated with flow rate, applied ICP power and inlet precursor fraction are discussed. While the spatial distribution of plasma produced radical species can have significant impact on the NP growth process, the NP transport dynamics are what ultimately dictates the growth environment that is unique to each particle and so determines their final dimension and composition. The key to optimizing reactor conditions involves controlling the spatial density of growth species and plasma profile as a means to tailor particle trapping dynamics suitable to produce CSNPs for a specific application.

36 MATERIALS SCIENCE↗

NASA NTRS1992

SiC particles from asymptotic giant branch stars - Mg burning and the s-process

The question of whether isotopically anomalous SiC particles found in meteorites originate in AGB stars is addressed. It is shown that if the peak helium shell flash temperatures of massive (6-9 solar masses) stars are about 10 percent larger than they are normally assumed to be, alpha particle reactions with the magnesium will become significant. Then the (Mg-29)(alpha, n)Si-29 reaction produces a large excess of Si-29. With a light element nuclear reaction network, the evolution of the silicon isotopic composition during AGB evolution is calculated. It is found that the experimentally determined correlation between excess Si-29 and excess Si-30 in SiC particles from carbonaceous chondrites can indeed be naturally produced in this way. It is suggested that if the large isotopically anomalous SiC particles carrying nearly pure-process krypton and xenon do indeed originate in AGB stars, those stars were massive and had peak shell flash temperatures near 450 KM.

Brown, Lawrence E.↗

DOE OSTI2025

Spatial and chemical heterogeneity in aqueous Zn/MnO 2 batteries: role of Zn and Mn containing complexes

Aqueous Zn/MnO 2 batteries are a promising, safe alternative for grid-scale energy storage, owing to their environmentally safe and low-cost nature. The dissolution–deposition reaction mechanism in a mild aqueous pH regime has recently gained significance due to its relevance in battery design. Comprehending both the specific locations and the way reaction progresses is crucial for efficient batteries. This study demonstrates that Zinc Hydroxy Sulfate (ZHS) formed during discharge primarily near the dissolved MnO2 particles. Acting as a host for charge reactants in subsequent cycles, the charge product morphology was visualized using operando X-ray fluorescence microscopy. After ∼400 hours of cycling, capacity fade was linked to the formation of a Zn–Mn core–shell phase which is attributed to an irreversible core phase in the electrode, visualized through three-dimensional chemical mapping. Altogether, this research underscores the importance of understanding local morphological evolution in designing electrodes and chemistries for advanced grid-scale energy storage technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Asymmetric nanoparticle oxidation observed in-situ by the evolution of diffraction contrast

Abstract The use of transmission electron microscopy (TEM) to observe real-time structural and compositional changes has proven to be a valuable tool for understanding the dynamic behavior of nanomaterials. However, identifying the nanoparticles of interest typically require an obvious change in position, size, or structure, as compositional changes may not be noticeable during the experiment. Oxidation or reduction can often result in subtle volume changes only, so elucidating mechanisms in real-time requires atomic-scale resolution or in-situ electron energy loss spectroscopy, which may not be widely accessible. Here, by monitoring the evolution of diffraction contrast, we can observe both structural and compositional changes in iron oxide nanoparticles, specifically the oxidation from a wüstite-magnetite (FeO@Fe 3 O 4 ) core – shell nanoparticle to single crystalline magnetite, Fe 3 O 4 nanoparticle. The in-situ TEM images reveal a distinctive light and dark contrast known as the ‘Ashby-Brown contrast’, which is a result of coherent strain across the core – shell interface. As the nanoparticles fully oxidize to Fe 3 O 4 , the diffraction contrast evolves and then disappears completely, which is then confirmed by modeling and simulation of TEM images. This represents a new, simplified approach to tracking the oxidation or reduction mechanisms of nanoparticles using in-situ TEM experiments.

36 MATERIALS SCIENCE↗

NASA NTRS1985

The Crab Nebula and related supernova remnants; Proceedings of the Workshop, George Mason University, Fairfax, VA, October 11, 12, 1984

Papers are presented on the Crab Nebula's composition, helium distribution, outer structure and jet, and evolution. Attention is given to line emission from supernova remnants and charge transfer reactions, a magnetohydrodynamic model of the Crab Nebula and its radiation, inferences made using data on the pulsed flux from the crab pulsar, a new interpretation of the crab pulsar X-ray interpulse radiation, and evolutionary models of the Crab Nebula's progenitor. Other topics include the evolution of the centimeter flux of 3C58 and the Crab Nebula, a search for a shock wave around the Crab Nebula, high resolution radio studies of the Crab Nebula, supernova shell structure, and the nature of the remnant 0540-693 and its implications for the study of crablike remnants. Papers are also presented on X-ray observations of: Crab-like remnants, the Crab Nebula, the Vela X region, W28, and 3C400.2. Other papers include the 50 millisecond pulsar in the Large Magellanic Cloud and the X-ray pulse emission mechanism, optical emission from the plerionic core of CTB 80, and one-arcminute resolution observations of W50.

Kafatos, M. C.↗

NASA NTRS1996

Analysis of IUE Observations of Supernovae

This program supported the analysis of IUE observations of supernovae. One aspect was a Target-of-Opportunity program to observe bright supernovae which was applied to SN 1993J in M81, and another was continuing analysis of the IUE data from SN 1987A. Because of its quick response time, the IUE satellite has continued to provide useful data on the ultraviolet spectra of supernovae. Even after the launch of the Hubble Space Telescope, which has much more powerful ultraviolet spectrometers, the IUE has enabled us to obtain early and frequent measurements of ultraviolet radiation: this information has been folded in with our HST data to create unique observations of supernova which can be interpreted to give powerful constraints on the physical properties of the exploding stars. Our chief result in the present grant period was the completion of a detailed reanalysis of the data on the circumstellar shell of SN 1987A. The presence of narrow high-temperature mission lines from nitrogen-rich gas close to SN 1987A has been the principal observational constraint on the evolution of the supernova's progenitor. Our new analysis shows that the onset of these lines, their rise to maximum, and their subsequent fading can be understood in the context of a model for the photoionization of circumstellar matter.

Kirshner, Robert P.↗

DOE OSTI2024

High-Fidelity and High-Performance Computational Simulations for Rapid Design Optimization of Sulfur Thermal Energy Storage

Industrial process heating (IPH) accounts for approximately 70% of US manufacturing energy use and is primarily produced by fossil fuel combustion. Approximately 1500 TWht (approximately 60%) of IPH demand is in the temperature range of 100-300. Industrial applications in this temperature range include drying, hydrothermal processing, thermal enhanced oil recovery, food and beverage, bioethanol production, etc. Cost-effective thermal energy storage (TES) that increases the utilization of waste and renewable heat (solar, geothermal, etc.) could provide significant energy savings and reliable heat sources, decrease emissions, and increase US manufacturing competitiveness through reductions in fuel consumption. TES development has historically been dominated by technologies suitable for deployment with concentrating solar power (CSP). State-of-the-art thermal storage deployed commercially with power tower CSP plants uses a 60%/40% NaNO3/KNO3 molten salt and operates between temperatures of approximately 280 degrees Celsius and 570 degrees Celsius using a two-tank configuration. However, these nitrate salts are unsuitable for operation outside of this temperature range due to a high freezing point of approximately 220 degrees Celsius, and limits on high-temperature salt stability and corrosion resistance of containment alloys. Other materials being investigated for TES include those based on: (1) sensible energy storage (various molten salt compositions, inert solid particles, rocks or pebble beds, sulfur, water, concrete, graphite, etc.), (2) latent energy storage in materials that undergo solid-liquid phase change at relevant temperatures (organic materials for low-temperature applications, inorganic salts and/or metals for high-temperature applications), or (3) thermochemical energy storage (hydrides, hydroxides, carbonates, metal oxides, etc.). The application temperature and challenges pertaining to storage material and/or containment cost, energy density, long-term thermal and cyclic stability, and charge/discharge heat transfer effectiveness drive material selection for a given IPH or electricity generation application. Sulfur is a cheap commodity at $80/ton compared to $1100 - 1300/ton for conventional salts. When using a metric of storage cost per kWh, sulfur costs around 2-3 $/kWh. Previous sulfur TES development focused on high temperature (>600 degrees) concentrated solar power applications with sulfur encapsulated in pipes and flow of gaseous HTF (air) in the shell side. However, for lower-temperature IPH applications in the range of approximately 100-300 degrees Celsius Element 16 adopted a compact and scalable TES design with molten sulfur in the shell and HTF pipes submerged in the molten sulfur bath. The low-cost molten sulfur TES for dispatchable IPH has deployment potential for broad applications. The spatial and temporal evolution of the HTF and sulfur temperature is critical to the TES system performance, and thus detailed modeling can improve understanding of the performance and facilitate design improvements. Using high performance computing and computational fluid dynamics (CFD) a low-cost molten sulfur thermal energy storage (TES) system for industrial process heating (IPH) applications was developed. The unique challenges in CFD modeling of sulfur TES are the sharp property changes of sulfur relevant to the working temperatures. Above 159, liquid sulfur undergoes polymerization, and the viscosity of sulfur rapidly increases by several orders of magnitude between 159 degrees Celsius and 188 degrees Celsius, followed by a decrease in viscosity beyond 188 degrees Celsius due to thermal bound dissociation. In addition, various concentrations of H2S impurities can also modify sulfur viscosity. This numerical challenge is especially relevant to transient simulation of the sulfur TES charging and discharging processes as the extreme property variations limit the applicability of traditional heat transfer correlations. Transient CFD simulations including the temperature-dependent sulfur properties and geometric complexity of the TES design were used to predict the effect of natural convection during charging and discharging on the heat transfer process, sulfur temperature uniformity, charge/discharge rates, and performance of the storage devices. The CFD model was validated with experimental results for a full charge and discharge cycle. The work will show 3D and 2D simulation comparisons aimed to facilitate rapid design iterations and a machine learning based design optimization approach.

CFD↗

NASA NTRS2000

Columbia University Participation in the Infrared Space Observatory (ISO) Guest Obs. Program: Evolution of Near-Infrared Lines from the Formation of Supernova Remnant 1987A

The goal of this project is to determine the mass loss history of a sample of seven mass losing Asymptotic Giant Branch stars. This is done by observing their circumstellar dust shells which contain a record of the most recent mass loss history. The further away from the star we are able to detect this increasingly fainter dust emission the further back we can look into the mass loss history.

Crotts, Arlin P. S.↗

DOE OSTI2023

The Effects of Shallow Cumulus Cloud Shape on Interactions Among Clouds and Mixing With Near-Cloud Environments

Cloud lifecycles are influenced by interactions among clouds and mixing with cloud-free environments. Cloud shapes dictate the length of cloud boundaries, which affects these interactions. This study uses a large eddy simulation to examine the relationships between the shallow cumulus cloud shapes, processes at their boundaries, and lifecycles. To characterize the shape of clouds, two metrics are newly defined: one reflects the overall horizontal cloud shape, and the other defines the cloud edge irregularity. Simulated clouds experience increased irregularity, but little changes in aspect ratio. Irregularity-driven cloud perimeter growth strongly indicates cloud splitting, with a more pronounced effect than aspect ratio-driven perimeter growth. Smaller cloud-shell gradients of properties across cloud boundaries are associated with more irregular clouds, suggesting enhanced mixing of clouds with the cloud-free environment. These findings indicate that the shallow cumulus evolution is partly driven by the irregularity of the cloud edge through lateral mixing and cloud splitting.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1972

Cooling and evolution of a supernova remnant.

Discussion of the structure, evolution, and cooling of an old supernova remnant, aimed at providing a theoretical framework for relating remnants with similar energies and environments but of different ages. Discussed evolution details include the Sedov-Taylor blast wave, the electron-ion equipartition and thermal conduction, the temperature sag and the dynamics in the process of transition to a dense shell, and the history of remnant luminosity.

Cox, D. P.↗

NASA NTRS1987

Study of pickup of cometary ions in turbulent solar winds

The influence of moderately strong magnetic disturbances on the ion pickup process near a comet is studied by a test-particle method. The research is motivated by recent observations with ICE and Giotto at Giacobini-Zinner and Halley. In this numerical study, the intrinsic hydromagnetic turbulence is modelled based on the Giotto and ICE data. The time evolution of the distribution function of the newborn ions is investigated. It is found that, when the level of the intrinsic turbulence is sufficiently high, the pickup ions can form a shell distribution function rapidly. The typical time scale for such a process is of the order of a couple of ion gyroperiods. On the other hand, if the turbulence is not strong, the pickup ions usually form an incomplete shell in the initial stage. The results seem to be consistent with available observations.

Wu, C. S.↗