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At least 721 records · Page 40

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DOE OSTI2023

Optimizing hierarchical membrane/catalyst systems for oxidative coupling of methane using additive manufacturing

The advantage of a membrane/catalyst system in oxidative coupling of methane (OCM) compared to conventional reactive systems is that by introducing oxygen to the OCM catalytic sites through a membrane, parasitic gas phase reactions of O 2 (g), responsible for lowering product selectivity, can be avoided. The design and fabrication of membrane/catalyst systems has, however, been hampered by low volumetric chemical conversion rates, high capital cost, and difficulties in codesigning membrane and catalyst properties to optimize the performance. We solve these issues by developing a dual-layer additive manufacturing process, based on phase inversion, to design, fabricate and optimize a hollow fiber membrane/catalyst system for OCM. We demonstrate the approach though a case study using BaCe 0.8 Gd 0.2 O 3-δ (BCG) as the basis of both the catalyst and separation layers. We show that by using the manufacturing approach we can codesign the membrane thickness and catalyst surface area so that the flux of oxygen transport through the membrane and methane activation rates in the catalyst layer match each other. Here, we demonstrate that this “rate matching” is critical for maximizing the performance, with the membrane/catalyst system significantly overperforming conventional reactor designs under identical conditions.

36 MATERIALS SCIENCE↗

NASA NTRS1993

Heterogeneous chemistry on Antarctic polar stratospheric clouds - A microphysical estimate of the extent of chemical processing

A detailed model of polar stratospheric clouds (PSCs), which includes nucleation, condensational growth. and sedimentation processes, has been applied to the study of heterogeneous chemical reactions. For the first time, the extent of chemical processing during a polar winter has been estimated for an idealized air parcel in the Antarctic vortex by calculating in detail the rates of heterogeneous reactions on PSC particles. The resulting active chlorine and NO(x) concentrations at first sunrise are analyzed with respect to their influence upon the Antarctic ozone hole using a photochemical model. It is found that the species present at sunrise are primarily influenced by the relative values of the heterogeneous reaction rate constants and the initial gas concentrations. However, the extent of chlorine activation is also influenced by whether N2O5 is removed by reaction with HCl or H2O. The reaction of N2O5 with HCl, which occurs rapidly on type 1 PSCs, activates the chlorine contained in the reservoir species HCl. Hence the presence and surface area of type 1 PSCs early in the winter are crucial in determining ozone depletion.

Drdla, K.↗

NASA NTRS1994

Annual variability of ozone along alpine hillsides

Over a period of more than two years (March 1989 till June 1991) ozone and nitrogen dioxide have been monitored along twelve alpine hillsides in the Austrian alps. The profiles had a height-resolution of 100 m and cover a range between 400 m and 1800 m asl, that is 100 m to 1100 m above the bottom of the valleys. They were situated in remote rural areas as well as in the vicinity of polluted urban and industrial areas. Both trace gases were monitored by means of integral chemical (SAM-surface active monitor) methods with a measuring cycle of two weeks. The concentration of ozone exhibits a substantial annual variation over the entire height range. In summer, highest ozone levels are observed near the ground and at the top of the mountains, whereas in winter the maxima are found mainly in the crest regions. The overall ozone burden shows a relative maximum near the temperature inversion layer in the valleys and an absolute maximum at the crest.

Putz, Erich↗

NASA NTRS2004

Electrochemical Reconstitution of Biomolecules for Applications as Electrocatalysts for the Bionanofuel Cell

Platinum-cored ferritins were synthesized as electrocatalysts by electrochemical biomineralization of immobilized apoferritin with platinum. The platinum cored ferritin was fabricated by exposing the immobilized apoferritin to platinum ions at a reduction potential. On the platinum-cored ferritin, oxygen is reduced to water with four protons and four electrons generated from the anode. The ferritin acts as a nano-scale template, a biocompatible cage, and a separator between the nanoparticles. This results in a smaller catalyst loading of the electrodes for fuel cells or other electrochemical devices. In addition, the catalytic activity of the ferritin-stabilized platinum nanoparticles is enhanced by the large surface area and particle size phenomena. The work presented herein details the immobilization of ferritin with various surface modifications, the electrochemical biomineralization of ferritin with different inorganic cores, and the fabrication of self-assembled 2-D arrays with thiolated ferritin.

Kim, Jae-Woo↗

NASA NTRS1996

Activity of Comet Hale-Bopp (1995 01) Beyond 6 AU From the Sun

The physical evolution of comet Hale-Bopp is investigated along the preperihelic arc of its orbit at heliocentric distances larger than 6 AU. The comet's considerable intrinsic brightness and activity are explained by the existence of a relatively larg area on its nucleus surface that is a resevoir of both carbon monoxide and dust particulates. Three recuring dust emission events observed in August-October 1995 are studied in some detail.

Hale-Bopp evolution carbon monoxide dust particula↗

NASA NTRSDate not supplied

Terrestrial Analogue Studies from ISRO’s Venus Mission Perspective: Polarimetric Radar Properties of Hawaiian Lava Flows

Detection of present and past volcanism on Venus is one of the major goals of the proposed ISRO’s Venus orbiter mission. The S-band, high-resolution (40 m/pixel) fully Polarimetric Synthetic Aperture Radar (PolSAR) instrument on this mission [1] may have the capabilities to detect volcanism within the mission lifetime using repeated PolSAR imagery, and possibly SAR Interferometry (InSAR, experimental mode). The global mapping efforts of Venus by Magellan mission has enabled comprehensive mapping of lava flows and indicated that Venus has an extensive history of volcanism, the ages of which are largely unknown (e.g. [2]). While Magellan radar emissivity data (e.g. [3, 4]) and Near Infrared emissivity data from VIRTIS [5] suggested the occurrence of recent episodes of volcanic activity (e.g. Maat Mons and Ganis Chasma), as well as the presence of stratigraphically young lava flows (e.g. Idunn Mons), measuring changes in radar backscatter amplitude alone to identify lava flows has many challenges. Although very large changes in the shape of the terrain can be observed in radar backscatter amplitude changes (e.g. [6]), smaller, or relatively flat lava flows are difficult to detect. Previous terrestrial studies suggest that PolSAR and InSAR techniques are very effective for mapping lava flows (e.g. [7-9]), and can be used when changes cannot be distinguished in radar backscatter images. We use the unvegetated lava flows on Hawaiʻi island as a terrestrial analogue to study Venus lava flows for the following reasons: (a) It is extensively studied at several wavelengths commonly used in remote sensing studies (including PolSAR and InSAR methods); and (b) it is a volcanically active area with new lava flows frequently covering older emplaced flows. To investigate the surface roughness, texture, and fine-grained mantling associated with Mauna Loa and Kilauea lava flows, we utilize C- and L-band PolSAR datasets obtained from RISAT-1A (EOS-4) and ALOS PALSAR missions respectively. In particular, we will use the quad-polarized backscatter and polarimetric parameters to characterize the texture of the terrestrial lava flows to understand whether the Venus crust is continuously disrupted during flow emplacement. While some previous studies (e.g. [10, 11]) suggested that surface roughness of most of the Venus flows is comparable to that of terrestrial pāhoehoe flows, other studies indicated that fractal dimensions of some large lava flows on Venus imply high eruption rates which favour the formation of a’a flows (e.g. [12]). We will also analyse the terrestrial flows for the presence/absence of pyroclastic mantling as radar-bright diffuse deposits near the summit regions of some coronae on Venus have been proposed to be young pyroclastics, and possible evidence of a renewed epoch of mantle volcanism that taps into deeper volatiles [13]. A recent study using EOS-4 RISAT-1 data of a part of fresh Mauna Loa lava flows (2022 eruption) emphasizes the ability of fully polarimetric SAR data to understand the diversity of physical properties (e.g. texture and morphology) associated with them (Sreejith et al. 2024); and we will apply similar methods to the PolSAR data obtained from ISRO’s Venus mission for our proposed objectives.

Sriram S Bhiravarasu↗

DOE OSTI2017

Method of operating a lithium-ion cell having a high-capacity cathode

A method of operating a lithium-ion cell comprising (a) a cathode comprising a carbon or graphitic material having a surface area to capture and store lithium thereon; (b) an anode comprising an anode active material; (c) a porous separator disposed between the two electrodes; (d) an electrolyte in ionic contact with the two electrodes; and (e) a lithium source disposed in at least one of the two electrodes to obtain an open circuit voltage (OCV) from 0.5 volts to 2.8 volts when the cell is made; wherein the method comprises: (A) electrochemically forming the cell from the OCV to either a first lower voltage limit (LVL) or a first upper voltage limit (UVL), wherein the first LVL is no lower than 0.1 volts and the first UVL is no higher than 4.6 volts; and (B) cycling the cell between a second LVL and a second UVL.

25 ENERGY STORAGE↗

DOE OSTI2019

Lithium-ion cell having a high-capacity cathode

Zhamu, Aruna↗

NASA NTRSDate not supplied

The Project “Analogs for Venus’ Geologically Recent Surfaces” (AVENGERS): A Comprehensive Database of Terrestrial Active Volcanoes for the Analysis of Ongoing Volcanism on Venus

The recently selected missions to Venus have opened a new era for the exploration of the Earth’s twin planet. As the Venus decade approaches, it is crucial to set the science goals for the future orbiting and in-situ investigations. One of the key science targets on Venus is certainly represented by the young topographic rises, which can be defined as the surface expression of underlying mantle plumes. These areas can be considered as the geologically youngest regions of Venus, being characterized by recent volcanic and tectonic activity. Studying areas of active volcanism and tectonism on Venus is crucial because it can reveal clues on the geologic past of the planet, as well as provide information about the volatile content of its interior and about the formation of its dense atmosphere. To this regard, the Project “Analogs for VENus’ GEologically Recent Surfaces” (AVENGERS) aims to build a database of Terrestrial analog sites for the analysis and identification of recent and possibly ongoing volcanic as well as tectonic activity on Venus to be investigated by the future missions. The Project AVENGERS will be a powerful tool for allowing a more efficient exploitation of the wealth of data to be provided by the future investigations of Venus during the upcoming decade.

P D Incecco↗

DOE OSTI2018

Correlating the electrocatalytic stability of platinum monolayer catalysts with their structural evolution in the oxygen reduction reaction

Platinum monolayer (Pt ML ) core–shell electrocatalysts for the oxygen reduction reaction (ORR) have attracted great attention because of their exceptional activity and stability for promising practical applications in fuel cells. In this paper, we describe our in-depth investigation of the relationship between the ORR activity and structure of the Pt ML /Pd/C catalyst during the stability test. By virtue of the rotating disk electrode technique, an accelerated degradation test with the potential window of 0.65 to 1.05 V was applied to the Pt ML /Pd/C to interrogate its long-term reliability in the ORR, the change of its electrochemical surface area, and its surface composition and components. The Pt ML /Pd/C catalyst displayed a volcano-like mass/dollar activity profile in the stability test up to 100k cycles. The overall loss of the activity was recorded to be as low as 17% of the initial value. The ORR activity increased in the initial 20k cycles because the freshly prepared Pt ML did not entirely encompass the whole Pd core, but it was integrated to a full coverage with a more stable configuration during the potential cycling owing to its self-healing property. Then, the activity decreased at a much slower rate than the standard Pt/C because the Pd–Pt core–shell structure due to its structural self-retaining property remained intact and impeded the electrochemical Ostwald ripening of the entire particles. Changes in the morphology and configuration of Pt ML were mapped by combining our experimental investigation with model analyses. Finally, the proposed self-healing and self-retaining mechanisms account for the structure-dependent stability in the ORR and play cornerstone roles in formulating ORR core–shell electrocatalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Seasonal forecasting skill for the High Mountain Asia region in the Goddard Earth Observing System

Seasonal variability of the global hydrologic cycle directly impacts human activities, including hazard assessment and mitigation, agricultural decisions, and water resources management. This is particularly true across the High Mountain Asia (HMA) region, where availability of water resources can change depending on local seasonality of the hydrologic cycle. Forecasting the atmospheric states and surface conditions, including hydrometeorologically relevant variables, at subseasonal-to-seasonal (S2S) lead times of weeks to months is an area of active research and development. NASA's Goddard Earth Observing System (GEOS) S2S prediction system has been developed with this research goal in mind. Here, we benchmark the forecast skill of GEOS-S2S (version 2) hydrometeorological forecasts at 1–3-month lead times in the HMA region, including a portion of the Indian subcontinent, during the retrospective forecast period, 1981–2016. To assess forecast skill, we evaluate 2 m air temperature, total precipitation, fractional snow cover, snow water equivalent, surface soil moisture, and terrestrial water storage forecasts against the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2) and independent reanalysis data, satellite observations, and data fusion products. Anomaly correlation is highest when the forecasts are evaluated against MERRA-2 and particularly in variables with long memory in the climate system, likely due to the similar initial conditions and model architecture used in GEOS-S2S and MERRA-2. When compared to MERRA-2, results for the 1-month forecast skill range from an anomaly correlation of R anom =0.18 for precipitation to R anom =0.62 for soil moisture. Anomaly correlations are consistently lower when forecasts are evaluated against independent observations; results for the 1-month forecast skill range from R anom =0.13 for snow water equivalent to R anom =0.24 for fractional snow cover. We find that, generally, hydrometeorological forecast skill is dependent on the forecast lead time, the memory of the variable within the physical system, and the validation dataset used. Overall, these results benchmark the GEOS-S2S system's ability to forecast HMA hydrometeorology.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2022

Emerging Modification Technologies of Lignin-based Activated Carbon toward Advanced Applications

Lignin-based activated carbon (LAC) is a promising high-quality functional material due to high surface area, abundant porous structure, and various functional groups. Modification is the most important step to functionalize LAC by altering its porous and chemical properties. Here, this Review summarizes the state-of-the-art modification technologies of LAC toward advanced applications. Promising modification approaches are reviewed to display their effects on the preparation of LAC. The multiscale changes in the porosity and the surface chemistry of LAC are fully discussed. Advanced applications are then introduced to show the potential of LAC for supercapacitor electrode, catalyst support, hydrogen storage, and carbon dioxide capture. Finally, the mechanistic structure-function relationships of LAC are elaborated. These results highlight that modification technologies play a special role in altering the properties and defining the functionalities of LAC, which could be a promising porous carbon material toward industrial applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1981

A microwave pressure sounder

A technique for the remote measurement of atmospheric surface pressure will be described. Such measurements could be made from a satellite in polar orbit and would cover many areas for which conventional meteorological data are not available. An active microwave instrument is used to measure the strength of return echoes from the ocean surface at a number of frequencies near the 60 GHz oxygen absorption band. Factors which affect the accuracy with which surface pressure can be deduced from these measurements will be discussed and an instrument designed to test the method by making measurements from an aircraft will be described.

Peckham, G. E.↗

NASA NTRS1973

Geological survey of Maryland using EREP flight data

The author has identified the following significant results. Underflight photography has been used in the Baltimore County mined land inventory to determine areas of disturbed land where surface mining of sand and ground clay, or stone has taken place. Both active and abandoned pits and quarries were located. Aircraft data has been used to update cultural features of Calvert, Caroline, St. Mary's, Somerset, Talbot, and Wicomico Counties. Islands have been located and catalogued for comparison with older film and map data for erosion data. Strip mined areas are being mapped to obtain total area disturbed to aid in future mining and reclamation problems. Coastal estuarine and Atlantic Coast features are being studied to determine nearshore bedforms, sedimentary, and erosional patterns, and manmade influence on natural systems.

Weaver, K. N.↗

DOE OSTI2019

A new trick for an old support: Stabilizing gold single atoms on LaFeO 3 perovskite

Single-atom catalysts (SACs) have shown great potential for achieving superior catalytic activity due to maximizing metal efficiency. The key obstacle in developing SACs lies in the availability of supports that can stabilize SACs. Here we report the first successful development of single gold (Au) atom catalysts supported on high-surface-area hierarchical perovskite oxides. The resulting Au single-atoms are extremely stable at calcination temperatures up to 700 °C in air and under reaction conditions. A high catalytic activity for CO oxidation and distinct self-activating property were also achieved. Furthermore, evidenced by theoretical calculations and experimental studies including X-ray absorption fine structures and in situ Fourier-transform infrared spectra, the surface Au active sites are confirmed to be predominately positively charged. This study provides a generalizable approach to fabricating highly stable Au single-atom catalysts with tunable catalytic performance, and we anticipate that this discovery will facilitate new possibilities for the development of single atom catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Effects of calcining temperature on photocatalysis of g-C{sub 3}N{sub 4}/TiO{sub 2} composites for hydrogen evolution from water

Highlights: • TiO{sub 2} promotes melon to form at 400 °C, whereas it forms at 500 °C for only melamine. • The highest photocatalytic activity was achieved when calcination was performed at 400 °C. • Coordinated N−Ti−N bonds were formed in MA/TiO{sub 2} (400) and disappeared at high temperature. • The surface area decreased and the pore size increased with increasing of temperature. • Only MA/TiO{sub 2} (400) has a narrower band gap than pure g-C{sub 3}N{sub 4}. - Abstract: A composite of graphitic carbon nitride and TiO{sub 2} (g-C{sub 3}N{sub 4}/TiO{sub 2}) with enhanced photocatalytic hydrogen evolution capacity was achieved by calcining melamine and TiO{sub 2} sol-gel precursor. Characterization results reveal that heating temperature had a great influence on the structure, surface area and properties of the composites. Compared with the polycondensation of pure melamine, the presence of TiO{sub 2} precursor can promote the formation of melon at a low temperature. The highest photocatalytic activity of g-C{sub 3}N{sub 4}/TiO{sub 2}(400) was achieved when the calcination was performed at 400 °C, exhibiting H{sub 2} production rate of 76.25 μmol/h under UV–vis light irradiation (λ > 320 nm) and 35.44 μmol/h under visible light irradiation (λ > 420 nm). The highest photocatalytic performance of g-C{sub 3}N{sub 4}/TiO{sub 2}(400) can be attributed to: (1) the strong UV–vis light absorption due to the narrow bandgap caused by synergic effect of TiO{sub 2} and g-C{sub 3}N{sub 4}, (2) high surface area and porosity, (3) the effective separation of photo-generated electron-holes owing to the favorable heterojunction between TiO{sub 2} and g-C{sub 3}N{sub 4}.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Amphiphilic Baskets for Supramolecular Nanoarchitectures at Interfaces: Inverted Monolayer Formation on Water

Interfacial chemistry of molecular baskets remains poorly understood despite their promise for supramolecular applications of detection and sequestration of toxic molecules including those of illicit drugs, organophosphorus compounds, and anticancer agents. We present a fundamental investigation of the interfacial behavior of three amphiphilic supramolecular baskets (ASB 4, 8, and 12), having increasingly longer yet linear alkyl chains at the top of their bowl-shaped cavity. The studies were completed at the air−water interface to elucidate surface activity, interfacial stability, self-assembly, and monolayer organization that drive inverted monolayer formation, in which the molecular arms orient toward the aqueous phase in a configuration opposite to that typically observed for lipids. Herein, surface pressure−area isotherms of ASB 4, 8, 12, deposited on a water surface, were performed in tandem with nonequilibrium relaxation experiments to quantify surface activity, thermodynamic stability, and monolayer compressibility of the baskets’ monolayer assembly. Brewster angle microscopy enabled direct visualization of morphological evolution, aggregation, and packing at the interface. We show that systematic extension of the hydrocarbon arms, from four to 12 methylene groups, progressively modifies intermolecular packing, drives distinct two-dimensional aggregation pathways, and increases number densities at the air−water interface. Atomistic molecular dynamics simulations corroborate many of these experimentally observed trends and provide mechanistic detail on the cooperative roles of basket topology and interfacial concentration in regulating the hydration structure and dynamics within the cavities generated by surface-adsorbing baskets, consistent with observed variations in surface activity and packing. Our results establish how the topology of these unique supramolecules and their concentration govern interfacial organization and offer a rational framework for designing amphiphiles with predictable behavior at soft interfaces.

Hydrocarbons↗

DOE OSTI2019

Simultaneous activation and N-doping of hydrothermal carbons by NaNH 2 : An effective approach to CO 2 adsorbents

Synthesis of carbon materials with both large surface area and abundant heteroatoms is an important task in scientific research. Traditional approaches mostly proceed at extremely high temperature, and suffer from complex routes and/or expensive raw materials. NaNH 2 has been recently found to be able to not only etch C atoms to create nanochannels, but also substitute O species to introduce N species. In this work, an effective approach to N-doped porous carbons was realized by treating hydrothermal carbons (HTCs) with sodium amide (NaNH 2 ). The considerable amount of O species preserved in pristine HTCs enables the achievement in simultaneous activation and N-doping of HTCs by NaNH 2 at relatively moderate temperature (400~600 °C). The porous and chemical structure of NaNH 2 -treated HTCs were characterized systematically. Although the pristine HTCs are almost non-porous and N-free, the specific surface areas and total N contents of prepared NaNH 2 -treated HTCs reach 190~2430 m 2 /g and 0.78~6.57 wt.% respectively. Furthermore, the CO 2 capture performance of NaNH 2 -treated HTCs was also examined considering their highly porous and N-doped nature. Interestingly, NaNH2-treated HTCs exhibit high CO 2 capacities, large CO 2 /N 2 selectivities, fast CO 2 adsorption rate and excellent recyclability, endowing them with potential application as solid adsorbents for CO 2 capture.

CO2 adsorption↗