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At least 487 records · Page 27
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Surface anchoring requirements for vanadia clusters on titanium oxide surfaces and their impact on activity for oxidative dehydrogenation of ethanol

Titanium oxide site requirements for the anchoring of catalytically active forms of dispersed vanadia species are investigated. Using a series of oxygen-modified titanium nitride materials, we systematically modify the available vanadia-anchoring moieties on the titanium-bearing support surface. This strategy in turn results in a very narrow size distribution of well-dispersed vanadia clusters anchored on the support. This synthesis technique ensures that only highly dispersed vanadia is present on the catalyst surface even at nominal monolayer coverages. A deeper insight into the catalytic behavior for ethanol partial oxidation of the active vanadia species is obtained by comparing intrinsic kinetic and thermodynamic parameters of kinetically relevant reaction steps (heat of ethanol adsorption, hydrogen abstraction activation energy, and the energetics of catalyst reoxidation). In conclusion, it is found that these parameters are dependent on the relative amount of oxygen in the titanium-bearing support and the resulting distribution of vanadia species, which validates the premise of a potential participation of lattice oxygen atoms of the titania support into the catalytic activity of active vanadia species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

First-Principles Insights into the Thermocatalytic Cracking of Ammonia-Hydrogen Blends on Fe(110). 2. Kinetics

Ammonia (NH 3 ) is an energy-rich molecule that is routinely synthesized from nitrogen (N 2 ) and hydrogen (H 2 ). NH 3 ’s more favorable physical properties compared to H 2 suggests it may offer a way to more conveniently store, transport, and, when needed, extract H 2 via thermal decomposition. However, the high kinetic barrier and endoergicity to decompose to H 2 and N 2 require high temperatures. The standard reaction free energy indicates nearly 100% thermodynamic conversion to the diatomic molecules only at ~673 K and higher. However, even at these temperatures, a catalyst, e.g., iron (Fe), is needed for favorable kinetic conversion. Here, in this study, we explore via density functional theory the kinetics of NH 3 decomposition on the most stable facet of body-centered cubic Fe, namely, (110), under typical high-temperature and finite-pressure operando conditions. We predict coverage-dependent energetics of elementary surface reactions, often neglected in atomic-scale modeling. From these models, we find the recombinative desorption of adsorbed N as N 2 is rate-determining at 573.15–773.15 K and even at an extreme case of 1173.15 K. From microkinetic modeling, we find that the steady-state turnover frequencies (TOFs) for N 2 and H 2 generation rates (r$_{H_2}$) depend exponentially on temperature. The catalyst achieves a steady-state TOF of 36.4 s –1 and an r$_{H_2}$ of 0.107 μmol cm –2 s –1 for a feed of 1.8 bar NH 3 with 0.2 bar H 2 at 1173.15 K. However, at 773.15 K, with the same feed composition and velocity, the steady-state TOF and r$_{H_2}$ decrease to 0.14 s –1 and 4.10 × 10 –4 μmol cm –2 s –1 , respectively, as the process is significantly hindered by slow N 2 desorption. Although at first glance counterintuitive, our simulations suggest that surface modifications that reduce Fe’s reactivity toward NH x species should enhance its overall NH 3 decomposition activity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Mild and Selective Hydrogenation of Nitrate to Ammonia in the Absence of Noble Metals

Motivated by increased awareness about nitrate contamination of surface waters and its deleterious effects in human and animal health, we sought an alternative, non-noble metal catalyst for the chemical degradation of nitrate. First row transition metal phosphides recently emerged as excellent alternatives for hydrogen evolution and hydrotreating reactions. We demonstrate that a key member of this family, Ni 2 P, readily hydrogenates nitrate (NO 3 – ) to ammonia (NH 3 ) near ambient conditions with very high selectivity (96%). One of the few non-precious metal-based catalysts for this transformation, and among ca. 1% of catalysts with NH 3 selectivity, Ni 2 P can be recycled multiple times with limited loss of activity. Both nitrite (NO 2 – ) and nitric oxide (NO) intermediates are also hydrogenated. Density functional theory (DFT) indicates that—in the absence of a catalyst—nitrite hydrogenation is the reaction bottleneck. A variety of adsorbates (H, O, N, NO) induce surface reconstruction with top-layer Ni-rich surface stoichiometry. Critically, H saturation coverage on Ni 2 P(001) is only ca. 3 nm –2 , significantly less than that on Pd(111) and Ni(111) of ca. 15–18 nm –2 , which may play a key role in allowing coadsorption of NO x – . Here the ability of Earth-abundant, binary metal phosphides such as Ni 2 P to catalyze nitrate hydrogenation could transform and help us to better understand the basic science behind catalytic hydrogenation and, in turn, advance the next generation of oxyanion removal technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Evaporative water loss of 1.42 million global lakes

The evaporative loss from global lakes (natural and artificial) is a critical component of the terrestrial water and energy balance. However, the evaporation volume of these water bodies—from the spatial distribution to the long-term trend—is as of yet unknown. Here, using satellite observations and modeling tools, we quantified the evaporation volume from 1.42 million global lakes from 1985 to 2018. We find that the long-term average lake evaporation is 1500 ± 150 km 3 year -1 and it has increased at a rate of 3.12 km 3 year -1 . The trend attributions include an increasing evaporation rate (58%), decreasing lake ice coverage (23%), and increasing lake surface area (19%). While only accounting for 5% of the global lake storage capacity, artificial lakes (i.e., reservoirs) contribute 16% to the evaporation volume. Our results underline the importance of using evaporation volume, rather than evaporation rate, as the primary index for assessing climatic impacts on lake systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Vitrification of Hanford Tank 241-AP-107 with Recycled Condensate

During the vitrification of nuclear waste at the Hanford Waste Treatment and Immobilization Plant (WTP) – the primary mission of the U.S. Department of Energy Office of River Protection – the offgas condensate generated from the waste-to-glass conversion is currently planned to be concentrated by evaporation in the Effluent Management Facility (EMF). This concentrated condensate can then be recycled back to the incoming waste and vitrified. To test the recycle process, a test apparatus was designed to mimic the EMF evaporator and used to concentrate a volume of condensate that had been previously produced during the vitrification of Hanford tank 241-AP-107 (referred to herein as AP-107) waste in a continuous laboratory-scale melter (CLSM). The test apparatus successfully concentrated the AP-107 condensate by a factor of 10 while retaining over 90 % of the technetium-99 ( 99 Tc), Cs, and I inventory. A second portion of AP-107 waste was retrieved by Washington River Protection Solutions, LLC, given to Pacific Northwest National Laboratory, and combined with the AP-107 condensate concentrate after undergoing solids filtration and cesium removal by ion exchange. This combination served to approximate the recycling action to be performed at the WTP. After the addition of glass-forming chemicals (GFCs), the combined AP-107 waste and AP-107 condensate concentrate were processed in the CLSM to produce a glass, called AP-107-1R, that was designed to satisfy the WTP baseline requirements (Kim et al. 2012). During the 8.87 hours of processing, 7.27 kg of AP-107-1R glass were produced for an average glass production rate of 1739 kg m 2 d -1 . Compared to the previous run in the CLSM without recycled condensate, the run with the recycle had a greater average glass production rate, but the rate was within the potential range of variability when processing melter feeds with similar composition in the CLSM. The glass produced from the AP-107 recycle run in the CLSM was within 10 % of the target AP-107-1R glass composition with respect to the primary glass components. Analysis of the minor component impurities revealed that their content in the glass product had approached their nominal target after 2 turnovers of the glass inventory in the CLSM while the activity of the minor radionuclides was retained in the glass product. The 99 Tc and total cesium content in the combined AP-107 waste and recycled condensate were maintained at concentrations expected to be experienced at the WTP. During processing in the CLSM, at discrete sampling time periods, the target 99 Tc/Cs mass ratio in the glass formulation varied from 0.9 to 62.9. Across this range, the Cs retention in the glass ranged from 53 to 60 %, while the retention from the entire runtime totaled 68 %, values which align with Cs retention in other scaled melter systems while processing LAW melter feeds at 99 Tc/Cs mass ratios ranging from 1 to 100. The 99 Tc retention in the glass ranged from 22 to 32 %, primarily due to the cold-cap coverage on the glass melt surface, the area covered by reacting melter feed, varying from ~80 % to ~95 % during processing, demonstrating greater volatility of 99 Tc from the glass while more surface was exposed, as expected based on previous 99 Tc volatility studies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Understanding FLiNaK Salt Intrusion Behavior on Nuclear-Grade Graphite via Neutron Tomography

Graphite is an essential material as a neutron moderator in molten salt reactors (MSRs). To understand the impact of salt on the graphite structure to develop structural materials for MSRs, molten salt intrusion behavior on nuclear-grade graphite was studied. The graphite samples, IG-110 and PCEA, were tested for infiltration with LiF-NaF-KF (FLiNaK) at 750°C, 5 bar for 12 h, and, after the intrusion experiment, the graphite was analyzed by neutron imaging. The graphite and Li from FLiNaK showed great contrast in the neutron attenuation coefficient. Thus, the salt behavior in the graphite structure has been visualized for the first time without damaging the sample. The 3D image of the graphite was reconstructed after a neutron computed tomography scan, and the average salt coverage distribution of the XY surface in different depths was obtained from the reconstructed 3D images.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
NASA NTRS1971

Hydrologic Conditions Viewed by the Nimbus Meteorological Satellites

The unexploited value of the Nimbus meteorological sensor data relates to the satellites' ability for global, temporal, repetitive and uniform tonal and spatial coverage of the earth's surface. Examples are presented illustrating how synoptic views of large areas increase interpretive capability and enable focusing on large targets of interest. The effect of resolution of the Nimbus imaging systems on these observations is discussed, together with the assessment of the areal and temporal magnitude of changes observed by these systems. Two case studies are presented exemplifying the satellites' ability for repetitive observations enabling phenomena to be monitored under special conditions. One study deals with changes observed in the Antarctic ice conditions utilizing the Nimbus 2 and 3 television picture data. The other study deals with terrestrial changes in the Mississippi River Valley and the Niger River Valley (Africa), observed primarily in the 0.7 to 1.3 micron spectral band.

Rabchevsky, G. A.↗
NASA NTRS1973

Mariner Mars 9 stereophotogrammetry

Discussion of the equipment and orbital specifications of the Mariner Mars 9 spacecraft - a Martian orbiter which was placed in orbit on Nov. 14, 1971, for an expected 50-year stay and has made possible a practically 100% photographic coverage of the planet's surface. The orbit has a nominal 12-hr period, a nominal periapsis of 1300 km, and a nominal apoapsis of 18,000 km. Many of the outstanding topographic features of the planet have been covered by the convergent stereopairs carried by the orbiter. Theoretical considerations are set forth concerning the necessary instrument orientation and rotation requirements to achieve such performance levels in this extraterrestrial application of photogrammetry. The photogrammetric method used in this mission is assessed as useful in the evaluation of outstanding Martian features such as the mammoth volcano of the Nix Olympica region.

Benesh, M.↗
NASA NTRS1978

Outfall siting with dye-buoy remote sensing of coastal circulation

A dye-buoy remote sensing technique has been applied to estuarine siting problems that involve fine-scale circulation. Small hard cakes of sodium fluorescein and polyvinyl alcohol, in anchored buoys and low-windage current followers, dissolve to produce dye marks resolvable in 1:60,000 scale color and color infrared imagery. Lagrangian current vectors are determined from sequential photo coverage. Careful buoy placement reveals surface currents and submergence near fronts and convergence zones. The technique has been used in siting two sewage outfalls in Hampton Roads, Virginia: In case one, the outfall region during flood tide gathered floating materials in a convergence zone, which then acted as a secondary source during ebb; for better dispersion during ebb, the proposed outfall site was moved further offshore. In case two, flow during late flood was found to divide, with one half passing over shellfish beds; the proposed outfall site was consequently moved to keep effluent in the other half.

Munday, J. C., Jr.↗
NASA NTRS1983

Locating Small Leaks in Large Structures

Test tool for detecting minute leads in bimetal joints, welds, or other locations employs fine-control valve and hypodermic needle. Test item is connected in conventional manner to helium mass spectrometer tuned to read extremely small amounts of helium gas. Uniqueness of method is ability to detect tiny leaks, through surfaces, not discoverable by gross coverage of test structures by helium gas.

Lawler, W. F.↗
NASA NTRS1983

Forest Resource Information System (FRIS)

The technological and economical feasibility of using multispectral digital image data as acquired from the LANDSAT satellites in an ongoing operational forest information system was evaluated. Computer compatible multispectral scanner data secured from the LANDSAT satellites were demonstrated to be a significant contributor to ongoing information systems by providing the added dimensions of synoptic and repeat coverage of the Earth's surface. Major forest cover types of conifer, deciduous, mixed conifer-deciduous and non-forest, were classified well within the bounds of the statistical accuracy of the ground sample. Further, when overlayed with existing maps, the acreage of cover type retains a high level of positional integrity. Maps were digitized by a graphics design system, overlayed and registered onto LANDSAT imagery such that the map data with associated attributes were displayed on the image. Once classified, the analysis results were converted back to map form as a cover type of information. Existing tabular information as represented by inventory is registered geographically to the map base through a vendor provided data management system. The notion of a geographical reference base (map) providing the framework to which imagery and tabular data bases are registered and where each of the three functions of imagery, maps and inventory can be accessed singly or in combination is the very essence of the forest resource information system design.

Source record↗
NASA NTRS1994

The development and validation of command schedules for SeaWiFS

An automated method for developing and assessing spacecraft and instrument command schedules is presented for the Sea-viewing Wide Field-of-view Sensor (SeaWiFS) project. SeaWiFS is to be carried on the polar-orbiting SeaStar satellite in 1995. The primary goal of the SeaWiFS mission is to provide global ocean chlorophyll concentrations every four days by employing onboard recorders and a twice-a-day data downlink schedule. Global Area Coverage (GAC) data with about 4.5 km resolution will be used to produce the global coverage. Higher resolution (1.1 km resolution) Local Area Coverage (LAC) data will also be recorded to calibrate the sensor. In addition, LAC will be continuously transmitted from the satellite and received by High Resolution Picture Transmission (HRPT) stations. The methods used to generate commands for SeaWiFS employ numerous hierarchical checks as a means of maximizing coverage of the Earth's surface and fulfilling the LAC data requirements. The software code is modularized and written in Fortran with constructs to mirror the pre-defined mission rules. The overall method is specifically developed for low orbit Earth-observing satellites with finite onboard recording capabilities and regularly scheduled data downlinks. Two software packages using the Interactive Data Language (IDL) for graphically displaying and verifying the resultant command decisions are presented. Displays can be generated which show portions of the Earth viewed by the sensor and spacecraft sub-orbital locations during onboard calibration activities. An IDL-based interactive method of selecting and testing LAC targets and calibration activities for command generation is also discussed.

Woodward, Robert H.↗
NASA NTRS1998

Baseline Observations of Hemispheric Sea Ice with the Nimbus 7 Scanning Multichannel Microwave Radiometer

The Scanning Multichannel Microwave Radiometer (SMMR) on board the NASA Nimbus 7 satellite was designed to obtain data for sea surface temperatures (SSTs), near-surface wind speeds, sea ice coverage and type, rainfall rates over the oceans, cloud water content, snow water equivalent, and soil moisture. In this paper, I shall emphasize the sea ice observations and mention briefly some important SST observations. A prime factor contributing to the importance of SMMR sea ice observations lies in their successful integration into a long-term time series, presently being extended by observations from the series of Special Sensor Microwave/Imager (SSMI) on board the DOD/DMSP F8, Fl1, and F12 satellites. This currently constitutes a 19-year data set. Almost half of this was provided by the SMMR. Unfortunately, the 4-year data set produced earlier by the single-channel Electrically Scanned Microwave Radiometer (ESMR) was not successfully integrated into the SMMR/SSMI data set. This resulted primarily from the lack of an overlap period to provide intersensor adjustment, but also because of the large difference between the algorithms to produce ice concentrations and large temporal gaps in the ESMR data. The lack of overlap between the SeaSat and Nimbus 7 SMMR data sets was an important consideration for also excluding the SeatSat one, but the spatial gaps especially in the Southern Hemisphere daily SeaSat observations was another. The sea ice observations will continue into the future by means of the Advanced Microwave Scanning Radiometer (AMSR) on board the ADEOS II and EOS satellites due to be launched in mid- and late-2000, respectively. Analysis of the sea ice data has been carried out by a number of different techniques. Long-term trends have been examined by means of ordinary least squares and band-limited regression. Oscillations in the data have been examined by band-limited Fourier analysis. Here, I shall present results from a novel combination of Principal Component analysis and the recently-developed Empirical Mode Decomposition (EMD). In this method, the data are first separated into spatial and temporal parts, and then the temporal parts of the first few PCs are broken into intrinsic modes by the EMD method.

Gloersen, Per↗
NASA NTRS2001

Detection and Characterization of Imperfections in Composite Pressure Vessels

The thermographic evaluation of composite structures for delaminations, disbonds, inclusions, porosity and microcracking has proven to be a valuable asset in the field of nondestructive testing. Coupling large area coverage, variable sensitivity and minimal surface contact with a photographic type image representation of structural anomalies; thermography has become a primary inspection method for composite structures. Thermography works well for locating both surface and subsurface defects in most composite systems ranging in thickness of up to 0.25 inch (0.64 cm) or more. The thermographic method for inspection of composite structures typically involves applying an external source of heat to the structure and then recording the changes in the surface heat profile manifested by embedded defects or by material property variations. If these temperature variations are large enough and an infrared camera with sufficient sensitivity is used, then the material or structural abnormality can be detected and referred back to its source. Interpreting the information given in a thermogram, can be a difficult task under ideal circumstances and extremely challenging in a real world setting. Variables including depth, thermal conductivity, orientation and size of the abnormality can all have a great influence on how its heat pattern will be seen by the imager. The work discussed in this paper illustrates how the microstructure of several commonly found defects in composite structures relate to their thermographic image counterpart. Two test cases are studied herein, including a large graphite/epoxy RP-1 fuel tank and a graphite composite cryogenic fuel feedline. The structures used in this study were designed to serve as manufacturing proof of concept specimens and to undergo hydroburst testing to verify manufacturing practices and structural design. Prior to hydrostatic testing the structures underwent 100% thermographic evaluation to ensure that no manufacturing or handling damage was present. Due to a large inclusion found in the feedline, it was pulled from service and dissected without performing the hydroproof The thermographic indications found in the RP-1 tank were below critical limits so it underwent a complete hydroproof loading series and finally a hydroburst. Following the hydroburst samples were cut from the tank in regions where thermography had located damage before the test. These regions were thermographically and then were cross-sectioned and photomicrographed.

Walker, James L.↗
NASA NTRS2002

Retrieval Of Cloud Pressure And Chlorophyll Content Using Raman Scattering In GOME Ultraviolet Spectra

Reliable cloud pressure estimates are needed for accurate retrieval of ozone and other trace gases using satellite-borne backscatter ultraviolet (buv) instruments such as the global ozone monitoring experiment (GOME). Cloud pressure can be derived from buv instruments by utilizing the properties of rotational-Raman scattering (RRS) and absorption by O2-O2. In this paper we estimate cloud pressure from GOME observations in the 355-400 nm spectral range using the concept of a Lambertian-equivalent reflectivity (LER) surface. GOME has full spectral coverage in this range at relatively high spectral resolution with a very high signal-to-noise ratio. This allows for much more accurate estimates of cloud pressure than were possible with its predecessors SBUV and TOMS. We also demonstrate the potential capability to retrieve chlorophyll content with full-spectral buv instruments. We compare our retrieved LER cloud pressure with cloud top pressures derived from the infrared ATSR instrument on the same satellite. The findings confirm results from previous studies that showed retrieved LER cloud pressures from buv observations are systematically higher than IR-derived cloud-top pressure. Simulations using Mie-scattering radiative transfer algorithms that include O2-O2 absorption and RRS show that these differences can be explained by increased photon path length within and below cloud.

Atlas, Robert↗
NASA NTRSDate not supplied

International Satellite Cloud Climatology Project

The International Satellite Cloud Climatology Project (ISCCP) was established as the first project of the World Climate Research Programme (WCP-2) to collect and analyze satellite radiance measurements to infer the global distribution of cloud radiative properties and their diurnal and seasonal variations. The operational phase of ISCCP began in July 1983 and is currently planned to continue through June 2010. [Mission Objectives] To produce a global, reduced resolution, infrared and visible, calibrated and normalized radiance data set containing basic information on the radiative properties of the atmosphere from which cloud parameters can be derived. To stimulate and coordinate basic research on techniques for inferring the physical properties of clouds from the condensed radiance data set and to apply the resulting algorithms to derive and validate a global cloud climatology for improving the parameterization of clouds in climate models. To promote research using ISCCP data and contributing to improved understanding of the Earth's radiation budget (top of the atmosphere and surface) and hydrological cycle. [Temporal_Coverage: Start_Date=1983-07-01; Stop_Date=] [Spatial_Coverage: Southernmost_Latitude=-90; Northernmost_Latitude=90; Westernmost_Longitude=-180; Easternmost_Longitude=180].

Rossow, William B.↗