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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Enhanced Selectivity for C 2 H 4 Production from C 2 H 6 on Partially Chlorinated IrO 2 (110) Surfaces

Modifying metal oxide surfaces to limit their oxidizing activity can provide a means of improving catalytic selectivity toward the partial oxidation of light alkanes. Here, in this study, we investigated the oxidation of C 2 H 6 on Cl-modified IrO 2 (110) surfaces using temperature-programmed reaction spectroscopy (TPRS) and first-principles microkinetic modeling. We find that substituting Cl for O in the IrO 2 (110) surface enhances the selectivity for C 2 H 6 conversion to C 2 H 4 during TPRS by suppressing extensive oxidation to CO x products, while also either enhancing C 2 H 4 production or altering it to a lesser extent, depending on the initial C 2 H 6 coverage. The C 2 H 4 selectivity increased with increasing C 2 H 6 and Cl coverage, but reached a limiting value below 50%. The Cl coverage changed negligibly during C 2 H 6 oxidation, and the surface reactivity decreased only marginally for Cl coverages up to 0.5 ML (monolayer). TPRS simulations using a microkinetic model predict C 2 H 4 and CO x product yields as a function of the Cl coverage that agree closely with the experimental results. According to the simulations, C 2 H 6 conversion to C 2 H 4 occurs on Cl-IrO 2 (110) by the hydrogenation of C 2 H 3 * species adsorbed in blocked states, in which neighboring sites are occupied only by unreactive HO and Cl species. The microkinetic modeling shows that H-hopping away from surface HO groups provides a relatively efficient route for C 2 H 3 * to escape blocked configurations and dehydrogenate, and that this process can limit the C 2 H 4 selectivity on Cl-IrO 2 (110) under the conditions studied. Overall, our results demonstrate that Cl-substitution into IrO 2 (110) enhances the selectivity for C 2 H 4 production from C 2 H 6 and provides insights into the reaction mechanism that can guide strategies to further improve the C 2 H 4 selectivity.

IrO2↗
NASA NTRS2023

Decommissioning of Air Sparge System at Vertical Processing Facility, Solid Waste Management Unit 077 Implementation Report

This document discusses the decommissioning of the air sparge (AS) system at the Vertical Processing Facility (VPF), Solid Waste Management Unit 077 at Kennedy Space Center, Florida completed between January 30, 2023, and February 8, 2023. A 2005 Resource Conservation and Recovery Act Facility Investigation identified chlorinated volatile organic compound impacts at the site. Following assessment activities, an AS system was in operation intermittently from April 2012 through October 2017, when the system was permanently shutdown due to equipment failure. Trichloroethene and vinyl chloride remained above their groundwater cleanup target levels in several monitoring wells and the site was moved into the Industrial Area Long Term Monitoring Program. VPF continues to be sampled biennially; the most recent event was May 2022. Successful implementation of this decommissioning project will reduce the risk of accidental AS and soil vapor extraction well damage and will lower operating costs associated with maintaining obsolete AS systems. Decommissioning the AS system at VPF included vegetation clearing to access AS wells and associated piping, abandonment of all on site AS wells, temporary electrical outage, and site restoration. At the completion of demobilization and site restoration activities, the site was returned to its original or better than original condition.

Jason J Bublitz↗
NASA NTRS1975

Preferential concentration of certain elements in smaller aerosols emitted from aircraft engines

Aerosols from aircraft engines were collected with an eight-stage cascade sampler for a period of 24 h. The aerosol samples from each stage were analyzed for their elemental composition using the proton-induced X-ray emission (PIXE) technique. Seventeen elements (Si, P, S, Cl, K, Ca, Ti, V, Fe, Ni, Cu, Zn, Br, Sr, Nb, Sn, and Pb) were positively identified and quantitated at each stage. Six elements (S, Ca, Fe, Zn, Sn, and Pb) showed a fractional concentration increase with decreasing aerosol size. Similar, but less well-defined, trends were also observed for V and Ni. Silicon and chlorine, on the other hand, showed an opposite trend. Neutron-activation analysis of bulk aerosol samples collected every 2 h over the same period showed a correlation between concentration of Si, Ca, V, Ti, Zn, Br, and Sn and the density of air traffic at the airport. Analysis of the aviation-fuel samples by PIXE indicates that major fractions of Pb, Sn, Br, Zn, Ni, Fe, V, Ca, and S observed in these aerosol studies come from the aircraft engine exhaust.

Jolly, R. K.↗
NASA NTRS1980

Recirculating sprayer for fiber-filled paints

Recirculating paint sprayer applies spray of coarse filler in highly volatile solvent. Sprayer was developed for applying insulation material containing epxoy resin, glass fibers, and inert fillers suspended in chlorinated solvents. Sprayer resists abrasive action of fiberglass filler and chemical activity of solvent. Pump and position ensure more uniform pressure at spray gun without backpressure regulator, which tended to clog in old sprayer.

Major, R. K.↗
NASA NTRS1995

Cleaning without chlorinated solvents

Because of health and environmental concerns, many regulations have been passed in recent years regarding the use of chlorinated solvents. The Oak Ridge Y-12 Plant has had an active program to find alternatives for these solvents used in cleaning applications for the past 7 years. During this time frame, the quantity of solvents purchased has been reduced by 92 percent. The program has been a twofold effort. Vapor degreasers used in batch cleaning operations have been replaced by ultrasonic cleaning with aqueous detergent, and other organic solvents have been identified for use in hand-wiping or specialty operations. In order to qualify these alternatives for use, experimentation was conducted on cleaning ability as well as effects on subsequent operations such as welding, painting, and bonding. Cleaning ability was determined using techniques such as x-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) which are capable of examining monolayer levels of contamination on a surface. Solvents have been identified for removal of rust preventative oils, lapping oils, machining coolants, lubricants, greases, and mold releases. Solvents have also been evaluated for cleaning urethane foam spray guns, swelling of urethanes, and swelling of epoxies.

Thompson, L. M.↗
NASA NTRS1982

Water Filter

A compact, lightweight electrolytic water sterilizer available through Ambassador Marketing, generates silver ions in concentrations of 50 to 100 parts per billion in water flow system. The silver ions serve as an effective bactericide/deodorizer. Tap water passes through filtering element of silver that has been chemically plated onto activated carbon. The silver inhibits bacterial growth and the activated carbon removes objectionable tastes and odors caused by addition of chlorine and other chemicals in municipal water supply. The three models available are a kitchen unit, a "Tourister" unit for portable use while traveling and a refrigerator unit that attaches to the ice cube water line. A filter will treat 5,000 to 10,000 gallons of water.

Source record↗
NASA NTRS2022

General Services Administration Reclamation Yard, SWMU 010, 2021 Groundwater Monitoring Report

This report presents a summary of the groundwater monitoring activities that occurred in November and December 2021 at General Services Administration Reclamation Yard, Solid Waste Management Unit 010, located at the John F. Kennedy Space Center (KSC), Florida. The site is monitored under KSC’s Resource Conservation and Recovery Act Corrective Action Program. This approach also meets the requirements of Chapter 62-780, Florida Administrative Code. For the purposes of this report, two separate plumes, known as the Polychlorinated Biphenyl (PCB)/Volatile Organic Aromatic (VOA) Plume and the Chlorinated Volatile Organic Compound (VOC) Plume, were identified for this site. The contaminants of concern (COCs) for the PCB/VOA Plume consists of PCBs, 1,2,4-trichlorobenzene, and breakdown products of 1,2,4-trichlorobenzene. The COCs for the Chlorinated VOC Plume are tetrachloroethene, trichloroethene, cis-1,2-dichloroethene, and vinyl chloride. The activities presented in this report include two field events: (1) November 2021 – PCB/VOA Plume groundwater sampling via Direct Push Technology – 70 groundwater samples were collected from 10 locations at varying intervals; and (2) December 2021 – Site-wide semi-annual water level measurements of 54 monitoring wells, redevelopment of 5 monitoring wells, and sampling of 35 monitoring wells. Results for the PCB/VOA plume demonstrated COCs have not rebounded since the 2018 source removal, with groundwater cleanup target levels (GCTLs) exceeded in the 10-30 ft. below ground surface interval only. In the Chlorinated VOC plume area, there were no detections of COCs above a GCTL for at least the second consecutive sampling event for the sampled wells. Cleanup objectives have been met, and it is recommended that VOC monitoring be discontinued. Underground injection control parameters will continue to be monitored in three wells until those analytes return to background concentrations.

GSA Reclamation Yard↗
DOE OSTI2020

Halogenation-Dependent Effects of the Chlorosulfolipids of Ochromonas danica on Lipid Bilayers

The chlorosulfolipids are amphiphilic natural products with stereochemically complex patterns of chlorination and sulfation. Despite their role in toxic shellfish poisoning, potential pharmacological activities, and unknown biological roles, they remain understudied due to the difficulties in purifying them from natural sources. The structure of these molecules, with a charged sulfate group in the middle of the hydrophobic chain, appears incompatible with the conventional lipid bilayer structure. Questions about chlorosulfolipids remain unanswered partly due to the unavailability of structural analogues with which to conduct structure–function studies. Here, we approach this problem by combining enantioselective total synthesis and membrane biophysics. Using a combination of Langmuir pressure–area isotherms of lipid monolayers, fluorescence imaging of vesicles, mass spectrometry imaging, natural product isolation, small-angle X-ray scattering, and cryogenic electron microscopy, we show that danicalipin A (1) likely inserts into lipid bilayers in the headgroup region and alters their structure and phase behavior. Specifically, danicalipin A (1) thins the bilayer and fluidizes it, allowing even saturated lipid to form fluid bilayers. Lipid monolayers show similar fluidizing upon insertion of danicalipin A (1). Furthermore, we show that the halogenation of the molecule is critical for its membrane activity, likely due to sterically controlled conformational changes. Synthetic unchlorinated and monochlorinated analogues do not thin and fluidize lipid bilayers to the same extent as the natural product. Overall, this study sheds light on how amphiphilic small molecules interact with lipid bilayers and the importance of stereochemistry and halogenation for this interaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1983

El Chichon - Composition of plume gases and particles

Aircraft measurements were made of trace gases, atmospheric particles, and condensed acid volatiles in the plume of El Chichon volcano, Chiapas, Mexico, in November 1982. Hydrogen sulfide was the primary gaseous sulfur species in the plume at the time of collection. Concentrations of 28 elements were determined by neutron activation analysis of particulate material from the plume. The volatile elements sulfur, chlorine, arsenic, selenium, bromine, antimony, iodine, tungsten, and mercury were enriched relative to bulk pyroclastic material by factors of 60 to 20,000. Arsenic, antimony, and selenium were associated predominantly with small (not greater than 3 micrometer) particles. Calcium and sodium were present almost exclusively on larger particles and aluminum and manganese were bimodally distributed. Ashladen particulate material injected into the stratosphere during the early violent eruptions was enriched by factors of 10 to 30 relative to ash in some of the same elements observed in the quiescent plume.

Kotra, J. P.↗
NASA NTRS2011

Satellite Observations and Chemistry Climate Models - A Meandering Path Towards Better Predictions

Knowledge of the chemical and dynamical processes that control the stratospheric ozone layer has grown rapidly since the 1970s, when ideas that depletion of the ozone layer due to human activity were put forth. The concept of ozone depletion due to anthropogenic chlorine increase is simple; quantification of the effect is much more difficult. The future of stratospheric ozone is complicated because ozone is expected to increase for two reasons: the slow decrease in anthropogenic chlorine due to the Montreal Protocol and its amendments and stratospheric cooling caused by increases in carbon dioxide and other greenhouse gases. Prediction of future ozone levels requires three-dimensional models that represent physical, photochemical and radiative processes, i.e., chemistry climate models (CCMs). While laboratory kinetic and photochemical data are necessary inputs for a CCM, atmospheric measurements are needed both to reveal physical and chemical processes and for comparison with simulations to test the conceptual model that CCMs represent. Global measurements are available from various satellites including but not limited to the LIMS and TOMS instruments on Nimbus 7 (1979 - 1993), and various instruments on the Upper Atmosphere Research Satellite (1991 - 2005), Envisat (2002 - ongoing), Sci-Sat (2003 - ongoing) and Aura (2004 - ongoing). Every successful satellite instrument requires a physical concept for the measurement, knowledge of physical chemical properties of the molecules to be measured, and stellar engineering to design an instrument that will survive launch and operate for years with no opportunity for repair but providing enough information that trend information can be separated from any instrument change. The on-going challenge is to use observations to decrease uncertainty in prediction. This talk will focus on two applications. The first considers transport diagnostics and implications for prediction of the eventual demise of the Antarctic ozone hole. The second focuses on the upper stratosphere, where ozone is predicted to increase both due to chlorine decrease and due to temperature decrease expected as a result of increased concentrations Of CO2 and other greenhouse gases. Both applications show how diagnostics developed from global observations are being used to explain why the ozone response varies among CCM predictions for stratospheric ozone in the 21st century.

Douglass, Anne R.↗
NASA NTRS2024

Isotopic Evidence of Long-Lived Volcanism on Io

Jupiter’s moon Io hosts extensive volcanism, driven by tidal heating. The isotopic composition of Io’s inventory of volatile chemical elements, including sulfur and chlorine, reflects its outgassing and mass-loss history and thus records information about its evolution. We used submillimeter observations of Io’s atmosphere to measure sulfur isotopes in gaseous sulfur dioxide and sulfur monoxide, and chlorine isotopes in gaseous sodium chloride and potassium chloride. We find 34S/32S = 0.0595 ± 0.0038 (equivalent to δ34S = +347 ± 86‰), which is highly enriched compared to average Solar System values and indicates that Io has lost 94 to 99% of its available sulfur. Our measurement of 37Cl/35Cl = 0.403 ± 0.028 (δ37Cl = +263 ± 88‰) shows that chlorine is similarly enriched. These results indicate that Io has been volcanically active for most (or all) of its history, with potentially higher outgassing and mass-loss rates at earlier times.

Katherine De Kleer↗
NASA NTRS1961

Effect of Surface Preparation and Gas Flow on Nitrogen Atom Surface Recombination

The effects of surface preparation and gas flow on the recombination of nitrogen atoms at copper and platinum surfaces were determined. Atoms were generated by an electrodeless 2450-megacycle-per-second discharge, and their concentration was measured by gas-phase titration with nitric oxide. Test surfaces were either vacuum-evaporated films or spheres machined from bulk metal and cemented around small glass-bead thermistors. Heat released by recombination was measured as the difference in electrical energy required to maintain a given thermistor temperature with and without a catalytic surface exposed. Recombination coefficients measured at flow velocities of 1120, 1790, 2250, and 3460 centimeters per second and at pressures of 0.42 and 0.59 millimeter of mercury showed that flow conditions had no effect. The results were also independent of atom concentration. A rough indication of the temperature dependence was obtained; it was greater for copper than for platinum. Platinum films deposited on platinum or on glass had the same activity - about 3 percent of the atoms impinging recombined. With copper, however, the glass substrate greatly reduced the percent of atoms recombining over that of a bulk copper substrate where 4 percent of the impinging atoms recombined. This effect could be overcome by depositing a second film on top of the first. Bulk metal samples were subjected to various surface treatments including polishing, degreasing with a chlorinated hydrocarbon, washing with nitric acid, and rinsing with water. Polished, degreased platinum had low activity compared to an evaporated film, but nitric acid treatment made it equivalent. Polished, degreased copper was only slightly less active than a copper film; nitric acid etching decreased the activity still further, probably by preferentially exposing facets of low catalytic efficiency.

Prok, George M.↗
NASA NTRS1991

Future chlorine-bromine loading and ozone depletion

The prediction of future ozone requires three elements: (1) a scenario for the net emissions of chemically and radiatively active trace gases from the land and oceans; (2) a global atmospheric model that projects the accumulation of these gases; and (3) a chemical transport model that describes the distribution of ozone for a prescribed atmospheric composition and climate. This chapter, of necessity, presents models for all three elements and focuses on the following: (1) atmospheric abundance of chlorine and bromine in the form of halocarbons; and (2) the associated perturbations to stratospheric ozone.

Prather, Michael J.↗
NASA NTRS1991

Acridine orange staining reaction as an index of physiological activity in Escherichia coli

The assumption that the acridine orange (AO) color reaction may be used as an index of physiological activity was investigated in laboratory grown Escherichia coli. Spectrofluorometric observations of purified nucleic acids, ribosomes and the microscopic color of bacteriophage-infected cells stained with AO confirmed the theory that single-stranded nucleic acids emit orange to red fluorescence while those that are double-stranded fluoresce green in vivo. Bacteria growing actively in a rich medium could be distinguished from cells in stationary phase by the AO reaction. Cells from log phase appeared red, whereas those in stationary phase were green. However, this differentiation was not seen when the bacteria were grown in a minimal medium or when a variation of the staining method was used. Also, shifting bacteria in stationary phase to starvation conditions rapidly changed their AO staining reaction. Boiling and exposure to lethal concentrations of azide and formalin resulted in stationary-phase cells that appeared red after staining but bacteria killed with chlorine remained green. These findings indicate that the AO staining reaction may be suggestive of physiological activity under defined conditions. However, variables in staining and fixation procedures as well as uncertainties associated with mixed bacterial populations in environmental samples may produce results that are not consistent with the classical interpretation of this reaction. The importance of validating the putative physiological implications of this staining reaction is stressed.

NASA Discipline Number 04-10↗
DOE OSTI2022

Mechanistic Study of 1,2-Dichloroethane Hydrodechlorination on Cu-Rich Pt–Cu Alloys: Combining Reaction Kinetics Experiments with DFT Calculations and Microkinetic Modeling

Cu-rich Pt–Cu bimetallic catalysts are among the most promising candidates for actively catalyzing the hydrodechlorination of 1,2-dichloroethane (1,2-DCA) toward ethylene production. Combining reaction kinetics experiments with density functional theory (DFT) calculations and mean-field microkinetic modeling, we present a systematic mechanistic study for 1,2-DCA hydrodechlorination on Cu-rich Pt–Cu alloy catalysts. Our DFT (PBE+(TS+SCS)) results suggest that increasing Cu content in the Pt–Cu alloy destabilizes C 2 -species adsorption while stabilizing the binding of atomic chlorine. The reaction energetics of all the elementary steps in the 1,2-DCA reaction network were calculated on a Pt 1 Cu 3 (111) model surface. The DFT results were then used to construct a microkinetic model, and the model-predicted reaction rates were compared with our reaction kinetics experimental results on a Cu-rich SiO 2 -supported Pt–Cu alloy catalyst through a parameter estimation procedure. Both the reaction kinetics experiments and the microkinetic model after parameter adjustments yielded 100% selectivity to ethylene. The microkinetic model pointed to a reaction pathway involving two sequential chlorine-removal steps on the Pt–Cu alloy catalyst, a mechanism distinct from the one previously identified on pure Pt/SiO 2 catalysts, which involved an initial hydrogen-removal step. Adjustments to the DFT-derived parameters indicate the possible formation of chlorine-induced Cu-enriched surface sites during 1,2-DCA hydrodechlorination conditions, sites that are more active than those encountered in the bulk Pt 1 Cu 3 (111) alloy surface. Furthermore, our study offers valuable initial insights on the 1,2-DCA hydrodechlorination reaction mechanism and the nature of the active sites on PtCu bimetallic catalysts.

1,2-Dichloroethane↗
DOE OSTI2025

Bioremediation of Chlorinated Volatile Organic Compounds: DOE Experiences and Lessons Learned

From the mid-1980s to the present, the Department of Energy (DOE) has developed, tested, and deployed diverse bioremediation strategies for chlorinated volatile organic compounds (cVOCs). A systematic review of these projects after decades of activity provides an opportunity to identify crosscutting themes and lessons learned. The knowledge provided by a DOE bioremediation retrospective represents a resource to support current and future bioremediation operations, and future decisions related to cVOC bioremediation. This systematic review examined the design, objectives, performance and outcomes for remediation projects at DOE sites including Savannah River, Hanford, Idaho, Mound and Pinellas. The results were used to identify emergent themes to provide actionable insights. The bioremediation retrospective technical team first developed standardized criteria to support the systematic review. Then, the evaluation was performed using a sequential process that was informed by local technical experts who identified and provided the structured information that served as the basis for the evaluation. The participation of these experts was invaluable to the effort. Importantly, DOE cVOC bioremediation efforts were implemented based on the foundational knowledge developed by U.S. Department of Defense (DoD) strategic and applied environmental technology development and certification programs, as well as technical, policy and regulatory guidance from the U.S. Environmental Protection Agency (EPA), Interstate Technology and Regulatory Council (ITRC), U.S. Geological Survey (USGS), industry, and universities. To maximize the value of the DOE cVOC bioremediation retrospective, the systematic review strategy focused on identifying important DOE-specific experiences, trends and lessons learned that would extend the knowledge available from these other key entities.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1994

Solar proton effects on austral ozone during the final months of 1989

Intense solar activity during 1989 prompted six major particle events. Four of these occurred between August and December. Energetic solar protons are a natural source of ozone depletion due to the nitric oxides they produce in the polar atmospheres. In particular, modelling (Reid et al., 1991) of an event that peaked on October 20 (with greater than 10 MeV proton flux of 73000 particles sq cm s(exp -1) ster(exp -1) yields 55 percent column density enhancements of NO over the southern polar cap. Total column ozone data from the total ozone ,mapping spectrometer (TOMS) instrument aboard the Nimbus 7 satellite used at times when solar illumination facilitates measurements by TOMS over the entire southern polar regions. The impact of odd nitrogen enhancements on the spatial extent of low total column ozone and of the total ozone mass, over a region August to December. Comparisons are made with previous years (1984 to 1988) of moderate solar activity. The effect, if any, of these events on ozone during times of heterogeneous chlorine chemistry and dynamic processes is discussed.

Stephenson, Judy A. E.↗