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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Growth of Extra-Large Chromophore Supramolecular Polymers for Enhanced Hydrogen Production

The control of morphology in bioinspired chromophore assemblies is key to the rational design of functional materials for light harvesting. Here, we investigate here morphological changes in perylene monoimide chromophore assemblies during thermal annealing in aqueous environments of high ionic strength to screen electrostatic repulsion. We found that annealing under these conditions leads to the growth of extra-large ribbon-shaped crystalline supramolecular polymers of widths from about 100 nm to several micrometers and lengths from 1 to 10 μm while still maintaining a unimolecular thickness. This growth process was monitored by variable-temperature absorbance spectroscopy, synchrotron X-ray scattering, and confocal microscopy. The extra-large single-crystal-like supramolecular polymers are highly porogenic, thus creating loosely packed hydrogel scaffolds that showed greatly enhanced photocatalytic hydrogen production with turnover numbers as high as 13 500 over ~110 h compared to 7500 when smaller polymers are used. Our results indicate great functional opportunities in thermally and pathway-controlled supramolecular polymerization.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Activity of Cu-Al-oxo extra-framework clusters for selective methane oxidation on Cu exchanged zeolites

Cu-zeolites are able to directly convert methane to methanol via a 3-step process using O2 as oxidant. Among the different zeolite topologies, Cu-exchanged mordenite (MOR) shows the highest methanol yields, attributed to a preferential formation of active Cu-oxo species in its 8-MR pores. The presence of extra-framework or partially detached Al species entrained in the micropores of MOR leads to the formation of nearly homotopic redox active Cu-Al-oxo nanoclusters with the ability to activate CH4. Studies of the activity of these sites together with characterization by 27Al NMR and IR spectroscopy leads to the conclusion that the active species are located in the 8-MR side pockets of MOR and it consists of two Cu ions and one Al linked by O. This Cu-Al oxo cluster shows an activity per Cu in methane oxidation significantly higher than of any previ-ously reported active Cu-oxo species. In order to determine unambiguously the structure of the active Cu-Al-oxo cluster, we combine experimental XANES of Cu K- and L- edges, Cu K-edge HERFD-XANES and Cu K-edge EXAFS with TDDFT and AIMD-assisted simulations. Our results provide evidence of a [Cu2AlO3]2+ cluster exchanged on MOR Al pairs that is able to oxidize up to two methane molecules per cluster at ambient pressure.

Methane oxidation, Cu L3-edge XANES, HERFD, TDDFT,↗
DOE OSTI2023

Reining in Radium for Nuclear Medicine: Extra-Large Chelator Development for an Extra-Large Ion

Targeted α therapy (TAT) of soft-tissue cancers using the α particle-emitting radionuclide 223 Ra holds great potential because of its favorable nuclear properties, adequate availability, and established clinical use for treating metastatic prostate cancer of the bone. Despite these advantages, the use of 223 Ra has been largely overshadowed by other α emitters due to its challenging chelation chemistry. A key criterion that needs to be met for a radionuclide to be used in TAT is its stable attachment to a targeting vector via a bifunctional chelator. The low charge density of Ra 2+ arising from its large ionic radius weakens its electrostatic binding interactions with chelators, leading to insufficient complex stability in vivo. In this study, we synthesized and evaluated macropa-XL as a novel chelator for 223 Ra. It bears a large 21-crown-7 macrocyclic core and two picolinate pendent groups, which we hypothesized would effectively saturate the large coordination sphere of the Ra 2+ ion. The structural chemistry of macropa-XL was first established with the nonradioactive Ba 2+ ion using X-ray diffraction and X-ray absorption spectroscopy, which revealed the formation of an 11-coordinate complex in a rare anti pendent-arm configuration. Subsequently, the stability constant of the [Ra(macropa-XL)] complex was determined via competitive cation exchange with 223 Ra and 224 Ra radiotracers and compared with that of macropa, the current state-of-the-art chelator for Ra 2+ . A moderate log K ML value of 8.12 was measured for [Ra(macropa-XL)], which is approximately 1.5 log K units lower than the stability constant of [Ra(macropa)]. This relative decrease in Ra 2+ complex stability for macropa-XL versus macropa was further probed using density functional theory calculations. Additionally, macropa-XL was radiolabeled with 223 Ra, and the kinetic stability of the resulting complex was evaluated in human serum. Furthermore, although macropa-XL could effectively bind 223 Ra under mild conditions, the complex appeared to be unstable to transchelation. Collectively, this study sheds additional light on the chelation chemistry of the exotic Ra 2+ ion and contributes to the small, but growing, number of chelator development efforts for 223 Ra-based TAT.

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

Promotion of adsorptive and catalytic properties of zeolitic Brønsted acid sites by proximal extra-framework Si(OH) x groups

Steric confinement in zeolites influences the catalytic conversion of alkanes. For zeolitic Brønsted acid sites, proximate extra-framework species introduce additional confinement to the pore constraints, enhancing the catalytic activity of alkane cracking. Although extra-framework alumina has been the most studied, here we report the element-specific impact of silica species. Further, by grafting extra-framework silica species close to Brønsted acid sites in H-ZSM-5 zeolite, the binding of bases like pyridine and amines is strengthened via van der Waals interactions with their aryl or alkyl chains. Brønsted acid sites close to extra-framework silica achieve a higher reaction rate of protolytic cracking of n-pentane via enthalpic (unlike entropic, as with extra-framework alumina) stabilization of the transition state by 24–51 kJ mol −1 . The lower activation energy points to an earlier transition state than in the presence of extra-framework alumina, with a better stabilization of the carbonium ions in the transition state compared to the parent zeolite.

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

Inhibition of Pyruvate Kinase From Thermoanaerobacterium saccharolyticum by IMP Is Independent of the Extra-C Domain

The pyruvate kinase (PYK) isozyme from Thermoanaerobacterium saccharolyticum (TsPYK) has previously been used in metabolic engineering for improved ethanol production. This isozyme belongs to a subclass of PYK isozymes that include an extra C-domain. Like other isozymes that include this extra C-domain, we found that TsPYK is activated by AMP and ribose-5-phosphate (R5P). Our use of sugar-phosphate analogs generated a surprising result in that IMP and GMP are allosteric inhibitors (rather than activators) of TsPYK. We believe this to be the first report of any PYK isozyme being inhibited by IMP and GMP. A truncated protein that lacks the extra C-domain is also inhibited by IMP. A screen of several other bacterial PYK enzymes (include several that have the extra-C domain) indicates that the inhibition by IMP is specific to only a subset of those isozymes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

The impacts of Extra-tropical ENSO Precursors on Tropical Pacific Decadal-scale Variability

Abstract Off-equatorial wind anomalies on seasonal timescales from both the North and South Pacific, known as “precursors” of the El Niño Southern Oscillation (ENSO), have been shown to independently trigger the ENSO feedbacks in the tropics and its teleconnections to the extra-tropics. However, the impacts of ENSO precursors on Tropical Pacific Decadal-scale Variability (TPDV) is still not well understood and quantified. We show that the dynamic sequence from extra-tropical ENSO precursors to ENSO (tropics) to extra-tropical ENSO teleconnections is not only important for ENSO, but acts as a primary mechanism to filter (e.g. reddening) the low-frequency variability of the seasonal precursors into the decadal-scale variance of the Pacific basin, accounting for the largest fraction of the TPDV (~65%) and its phase. This process, which contrasts previous theories advocating for a TPDV generated internally in the tropics (e.g. ENSO residuals), is inherently unpredictable and not well reproduced in climate models and raises challenges for understanding and predicting the role of internal TPDV in future climate change scenarios.

Zhao, Yingying↗
DOE OSTI2025

Explaining the extra crystal-field mode in 𝐴 ⁢Ce ⁢𝑋 2 (𝐴 = K, Rb, Na; 𝑋 = O, S, Se, Te)

A growing list of Ce-based magnets have shown an extra and heretofore unexplained crystal electric field (CEF) mode at high energies. We describe a process whereby an optical phonon can produce a split CEF mode well above the phonon energy. We use density functional theory and point-charge model calculations to estimate the phonon distortions and coupling to model this effect in KCeO 2 , showing that it accounts for the extra CEF mode observed. Furthermore, this mechanism is generic and may explain the extra modes observed on a variety of Ce 3+ compounds.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Kinetic mixing, dark photons and extra dimensions. Part III. Brane localized dark matter

Extra dimensions have proven to be a very useful tool in constructing new physics models. In earlier work, we began investigating toy models for the 5-D analog of the kinetic mixing/vector portal scenario where the interactions of dark matter, taken to be, e.g., a complex scalar, with the brane-localized fields of the Standard Model (SM) are mediated by a massive U(1) D dark photon living in the bulk. These models were shown to have many novel features differentiating them from their 4-D analogs and which, in several cases, avoided some well-known 4-D model building constraints. However, these gains were obtained at the cost of the introduction of a fair amount of model complexity, e.g., dark matter Kaluza-Klein excitations. In the present paper, we consider an alternative setup wherein the dark matter and the dark Higgs, responsible for U(1) D breaking, are both localized to the ‘dark’ brane at the opposite end of the 5-D interval from where the SM fields are located with only the dark photon now being a 5-D field. The phenomenology of such a setup is explored for both flat and warped extra dimensions and compared to the previous more complex models.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Gravitational waves from primordial black hole evaporation with large extra dimensions

Abstract The spectra of gravitational waves from black hole evaporation generically peak at frequencies of order the Hawking temperature, making this signal ultra-high frequency for primordial black holes evaporating in the early universe. This motivates us to consider small black holes in theories with large extra dimensions, for which the peak frequency can be lowered substantially, since the true bulk Planck scaleM * can be much smaller than the effectiveM Pl . We study the emission of brane-localized gravitons during the Hawking evaporation of ultra-light primordial black holes in the context of theories with large extra dimensions, with the ultimate goal of computing the contribution to the stochastic gravitational wave background. To accurately model black hole evolution, we compute greybody factors for particles of spin-0, 1/2, 1, and 2 emitted on the brane and in the bulk, presuming the majority of emission proceeds during the Schwarzschild phase. We then compute the power spectrum and present day spectral density parameter for brane-localized gravitons contributing to a gravitational wave signal. We find that for an optimal choice of parameters, the peak frequency plateaus in the sub-MHz regime, within range of planned high-frequency gravitational wave detectors, making this scenario a target for detection once their sensitivity exceeds ΔN eff bounds.

Astronomy & Astrophysics↗
DOE OSTI2021

Dark Energy Camera photometry reveals extra-tidal stars around the Milky Way globular cluster NGC 6864 (M75)

ABSTRACT Globular clusters are prone to lose stars while moving around the Milky Way. These stars escape the clusters and are distributed throughout extended envelopes or tidal tails. However, such extra-tidal structures are not observed in all globular clusters, and yet there are no structural or dynamical parameters that can predict their presence or absence. NGC 6864 is an outer halo globular cluster with reported no observed tidal tails. We used Dark Energy Camera photometry reaching ∼4 mag underneath its main-sequence turnoff to confidently detect an extra-tidal envelope, and stellar debris spread across the cluster outskirts. These features emerged once robust field star filtering techniques were applied to the fainter end of the observed cluster main sequence. NGC 6864 is associated to the Gaia-Enceladus dwarf galaxy, among others 28 globular clusters. Up-to-date, nearly 64${{\ \rm per\,cent}}$ of them have been targeted looking for tidal tails and most of them have been confirmed to exhibit tidal tails. Thus, the present outcomes allow us to speculate on the possibility that Gaia-Enceladus globular clusters share a common pattern of mass loss by tidal disruption.

Piatti, Andrés E. (ORCID:0000000286790589)↗
DOE OSTI2021

Probing compactified extra dimensions with gravitational waves

We study the effect of compact extra dimensions on the gravitational wave luminosity and waveform. We consider a toy model, with a compactified fifth dimension, and matter confined on a brane. We work in the context of five-dimensional (5D) general relativity, though we do make connections with the corresponding Kaluza-Klein effective 4D theory. We show that the luminosity of gravitational waves emitted in 5D gravity by a binary with the same characteristics (same masses and separation distance) as a 4D binary is 20.8% less relative to the 4D case, to leading post-Newtonian order. The phase of the gravitational waveform differs by 26% relative to the 4D case, to leading post-Newtonian order. Such a correction arises mainly due to the coupling between matter and dilaton field in the effective 4D picture and agrees with previous calculations when we set black holes’ scalar charges to be those computed from the Kaluza-Klein reduction. The above corrections to the waveform and the luminosity are inconsistent with the gravitational-wave and binary pulsar observations, and they thus effectively rule out the possibility of such a simple compactified higher dimensions scenario. We also comment on how our results change if there are several compactified extra dimensions and show that the discrepancy with 4D general relativity only increases.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

A stable aluminosilicate zeolite with intersecting three-dimensional extra-large pores

Extra-large and intersecting pores Thermally stable zeolites with large pores, such as zeolite Y with 12-membered rings, are used for converting large molecules from petroleum into smaller, more useful hydrocarbons. Lin et al . report the synthesis of ZEO-1, a thermally stable zeolite with extra-large, 16-membered rings. The use of tricyclohexylmethylphosphonium as an organic structure–directing agent created a zeolite with a fully interconnected multidimensional framework and a very high specific surface area. —PDS

Science & Technology - Other Topics↗
DOE OSTI2021

Quantitative Evaluation of Top Coal Caving Methods at the Working Face of Extra‐Thick Coal Seams Based on the Random Medium Theory

Adopting an effective top coal caving method is the key to enhancing coal recovery and reducing gangue content for the fully mechanized top coal caving working face with extra‐thick coal seams. In this study, the movement of coal particles generated during top coal caving is considered to follow a normal distribution. Then, the caving body and coal‐rock settlement along the working face during the caving process are studied based on both the random media theory and probability theory. Accordingly, the optimal caving interval and caving sequences are determined, and a novel interval symmetrical coal caving method is proposed. The proposed method is systematically verified with results from physical similarity tests, and different caving methods are assessed by field tests. The results show the following: (1) The coal‐rock settlement and the caving body demonstrate clear axial symmetrical features along the working face; the size of the caving body increases as the caving height grows and its shape turns progressively from semicircular to semielliptical with a lower foot of the coal‐rock settlement. (2) The caving interval is derived using the sum of the radii of the coal‐rock settlement curves formed by the two largest caving bodies. (3) The symmetrical caving approach provides a symmetrical space for the subsequent movement of the broken top coal, which enables a uniform development of the caving body. (4) Compared with the traditional sequential coal caving method with the same number of supports, the interval symmetrical caving method results in a 21.7% of coal production increase, 17% caving rate promotion, and a shortened caving time by 23.4%. (5) The interval symmetrical caving method is found to improve the controllability of the caving process at the fully mechanized top coal caving working face. In general, this work presents a theoretical approach to select the optimal caving methods for the fully mechanized caving working face in extra‐thick coal seams for an improved production efficiency of the work face. The results of this study can also provide theoretical significance and referencing value for quantitative analyses of the coal caving methods for work faces with similar geological conditions.

Jiulin, Shi (ORCID:0000000155819062)↗
DOE OSTI2022

Extra-Cold EP Process at Fermilab

FNAL has established a cold Electro-Polishing (EP) method which maintains the outer surface temperature of cavity cell around 12~15°C during EP process. Cold EP has been applied on the various SRF cavities and contributed to achieve high RF performances with them. To investigate more feasibility and capability of EP at lower temperature, the FNAL EP temperature control tool was recently improved. Extra-cold EP process below 0°C at cavity cell region was successfully performed on 1.3 GHz 1-cell cavity. A compatible RF performance with cold EP method was also demonstrated during the cavity vertical testing. The details of extra-cold EP process and the cavity test results will be presented.

43 PARTICLE ACCELERATORS↗
DOE OSTI2025

Milky way bulge extra-tidal star survey: MWBest

The Milky Way Bulge Extra-Tidal Star Survey (MWBest) is a spectroscopic initiative aimed at identifying stars that have been tidally stripped from globular clusters in the inner regions of the Galaxy. As part of the Visiting Faculty Program at Fermilab, we have developed theoretical tools and simulations to compare against observed signatures of extra-tidal stars surrounding both bulge globular clusters (GCs) and low-luminosity clusters. By combining the spatial distributions of simulated stripped stars with new MWBest observations, we are gaining insight into the gravitational potential of the inner Galaxy and the role that bulge GCs may play in enriching the surrounding field star population. We further explore the hypothesis that some low-luminosity bulge GCs may in fact be dense clumps of debris, stripped from more massive GCs as they migrate inward due to dynamical friction.

Kunder, Andrea [Unlisted, US, WA]↗
DOE OSTI2022

Novel Mutant Alleles Reveal a Role of the Extra-Large G Protein in Rice Grain Filling, Panicle Architecture, Plant Growth, and Disease Resistance

Plant growth and grain filling are the key agronomical traits for grain weight and yield of rice. The continuous improvement in rice yield is required for a future sustainable global economy and food security. The heterotrimeric G protein complex containing a canonical α subunit (RGA1) couples extracellular signals perceived by receptors to modulate cell function including plant development and grain weight. We hypothesized that, besides RGA1, three atypical, extra-large GTP-binding protein (XLG) subunits also regulate panicle architecture, plant growth, development, grain weight, and disease resistance. Here, we identified a role of XLGs in agronomic traits and stress tolerance by genetically ablating all three rice XLGs individually and in combination using the CRISPR/Cas9 genome editing in rice. For this study, eight (three single, two double, and three triple) null mutants were selected. Three XLG proteins combinatorically regulate seed filling, because loss confers a decrease in grain weight from 14% with loss of one XLG and loss of three to 32% decrease in grain weight. Null mutations in XLG2 and XLG4 increase grain size. The mutants showed significantly reduced panicle length and number per plant including lesser number of grains per panicle compared to the controls. Loss-of-function of all individual XLGs contributed to 9% more aerial biomass compared to wild type (WT). The double mutant showed improved salinity tolerance. Moreover, loss of the XLG gene family confers hypersensitivity to pathogens. Our findings suggest that the non-canonical XLGs play important roles in regulating rice plant growth, grain filling, panicle phenotype, stress tolerance, and disease resistance. Genetic manipulation of XLG s has the potential to improve agronomic properties in rice.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

On the Nature of Extra-Framework Aluminum Species and Improved Catalytic Properties in Steamed Zeolites

Steamed zeolites exhibit improved catalytic properties for hydrocarbon activation (alkane cracking and dehydrogenation). The nature of this practically important phenomenon has remained a mystery for the last six decades and was suggested to be related to the increased strength of zeolitic Bronsted acid sites after dealumination. We now utilize state-of-the-art infrared spectroscopy measurements and prove that during steaming, aluminum oxide clusters evolve (due to hydrolysis of Al out of framework positions with the following clustering) in the zeolitic micropores with properties very similar to (nano) facets of hydroxylated transition alumina surfaces. The Bronsted acidity of the zeolite does not increase and the total number of Bronsted acid sites decreases during steaming. O 5 Al(VI)-OH surface sites of alumina clusters dehydroxylate at elevated temperatures to form penta-coordinate Al 1 O 5 sites that are capable of initiating alkane cracking by breaking the first C-H bond very effectively with much lower barriers (at lower temperatures) than for protolytic C-H bond activation, with the following reaction steps catalyzed by nearby zeolitic Bronsted acid sites. This explains the underlying mechanism behind the improved alkane cracking and alkane dehydrogenation activity of steamed zeolites: heterolytic C-H bond breaking occurs on Al-O sites of aluminum oxide clusters confined in zeolitic pores. Our findings explain the origin of enhanced activity of steamed zeolites at the molecular level and provide the missing understanding of the nature of extra-framework Al species formed in steamed/dealuminated zeolites.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Dark energy, extra dimensions, and the Swampland

Perhaps the greatest challenge for fundamental theories based on compactification from extra dimensions is accommodating a period of accelerated cosmological expansion. Previous studies have identified constraints imposed by the existence of dark energy for two overlapping classes of compactified theories: (1) those in which the higher dimensional picture satisfies certain metric properties selected to reproduce known low energy phenomenology; or (2) those derived from string theory assuming they satisfy the Swampland conjectures. For either class, the analyses showed that dark energy is only possible if it takes the form of quintessence. In this paper, we explore the consequences for theories that belong to both classes and show that the joint constraints are highly restrictive, leaving few options.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗